TY - JOUR A1 - Zhu, Hui A1 - Shprits, Yuri Y. A1 - Spasojevic, M. A1 - Drozdov, Alexander T1 - New hiss and chorus waves diffusion coefficient parameterizations from the Van Allen Probes and their effect on long-term relativistic electron radiation-belt VERB simulations JF - Journal of Atmospheric and Solar-Terrestrial Physics N2 - New wave frequency and amplitude models for the nightside and dayside chorus waves are built based on measurements from the Electric and Magnetic Field Instrument Suite and Integrated Science (EMFISIS) instrument onboard the Van Allen Probes. The corresponding 3D diffusion coefficients are systematically obtained. Compared with previous commonly-used (typical) parameterizations, the new parameterizations result in differences in diffusion rates that depend on the energy and pitch angle. Furthermore, one-year 3D diffusive simulations are performed using the Versatile Electron Radiation Belt (VERB) code. Both typical and new wave parameterizations simulation results are in a good agreement with observations at 0.9 MeV. However, the new parameterizations for nightside chorus better reproduce the observed electron fluxes. These parameterizations will be incorporated into future modeling efforts. KW - Inner magnetosphere KW - Radiation belts KW - Chorus waves KW - Diffusion coefficients KW - VERB code Y1 - 2019 U6 - https://doi.org/10.1016/j.jastp.2019.105090 SN - 1364-6826 SN - 1879-1824 VL - 193 PB - Elsevier CY - Oxford ER - TY - THES A1 - Kerutt, Josephine Victoria T1 - The high-redshift voyage of Lyman alpha and Lyman continuum emission as told by MUSE T1 - Die Reise der Lyman alpha- und Lyman Kontinuumsemission bei hoher Rotverschiebung erzählt von MUSE N2 - Most of the matter in the universe consists of hydrogen. The hydrogen in the intergalactic medium (IGM), the matter between the galaxies, underwent a change of its ionisation state at the epoch of reionisation, at a redshift roughly between 6>z>10, or ~10^8 years after the Big Bang. At this time, the mostly neutral hydrogen in the IGM was ionised but the source of the responsible hydrogen ionising emission remains unclear. In this thesis I discuss the most likely candidates for the emission of this ionising radiation, which are a type of galaxy called Lyman alpha emitters (LAEs). As implied by their name, they emit Lyman alpha radiation, produced after a hydrogen atom has been ionised and recombines with a free electron. The ionising radiation itself (also called Lyman continuum emission) which is needed for this process inside the LAEs could also be responsible for ionising the IGM around those galaxies at the epoch of reionisation, given that enough Lyman continuum escapes. Through this mechanism, Lyman alpha and Lyman continuum radiation are closely linked and are both studied to better understand the properties of high redshift galaxies and the reionisation state of the universe. Before I can analyse their Lyman alpha emission lines and the escape of Lyman continuum emission from them, the first step is the detection and correct classification of LAEs in integral field spectroscopic data, specifically taken with the Multi-Unit Spectroscopic Explorer (MUSE). After detecting emission line objects in the MUSE data, the task of classifying them and determining their redshift is performed with the graphical user interface QtClassify, which I developed during the work on this thesis. It uses the strength of the combination of spectroscopic and photometric information that integral field spectroscopy offers to enable the user to quickly identify the nature of the detected emission lines. The reliable classification of LAEs and determination of their redshifts is a crucial first step towards an analysis of their properties. Through radiative transfer processes, the properties of the neutral hydrogen clouds in and around LAEs are imprinted on the shape of the Lyman alpha line. Thus after identifying the LAEs in the MUSE data, I analyse the properties of the Lyman alpha emission line, such as the equivalent width (EW) distribution, the asymmetry and width of the line as well as the double peak fraction. I challenge the common method of displaying EW distributions as histograms without taking the limits of the survey into account and construct a more independent EW distribution function that better reflects the properties of the underlying population of galaxies. I illustrate this by comparing the fraction of high EW objects between the two surveys MUSE-Wide and MUSE-Deep, both consisting of MUSE pointings (each with the size of one square arcminute) of different depths. In the 60 MUSE-Wide fields of one hour exposure time I find a fraction of objects with extreme EWs above EW_0>240A of ~20%, while in the MUSE-Deep fields (9 fields with an exposure time of 10 hours and one with an exposure time of 31 hours) I find a fraction of only ~1%, which is due to the differences in the limiting line flux of the surveys. The highest EW I measure is EW_0 = 600.63 +- 110A, which hints at an unusual underlying stellar population, possibly with a very low metallicity. With the knowledge of the redshifts and positions of the LAEs detected in the MUSE-Wide survey, I also look for Lyman continuum emission coming from these galaxies and analyse the connection between Lyman continuum emission and Lyman alpha emission. I use ancillary Hubble Space Telescope (HST) broadband photometry in the bands that contain the Lyman continuum and find six Lyman continuum leaker candidates. To test whether the Lyman continuum emission of LAEs is coming only from those individual objects or the whole population, I select LAEs that are most promising for the detection of Lyman continuum emission, based on their rest-frame UV continuum and Lyman alpha line shape properties. After this selection, I stack the broadband data of the resulting sample and detect a signal in Lyman continuum with a significance of S/N = 5.5, pointing towards a Lyman continuum escape fraction of ~80%. If the signal is reliable, it strongly favours LAEs as the providers of the hydrogen ionising emission at the epoch of reionisation and beyond. N2 - Die Materie zwischen den Galaxien im Universum, das sogenannte intergalaktische Medium, besteht zum größten Teil aus Wasserstoff, welcher sich zusammensetzt aus einem Proton und einem Elektron. Etwa ~10^8 Jahre nach dem Urknall änderte sich der Ionisationszustand des Wasserstoffs im intergalaktischen Medium. Durch Strahlung wurden Proton und Elektronen getrennt, der Wasserstoff wurde ionisiert. Die Strahlung mit der nötigen Energie um Wasserstoff zu ionisieren nennt man Lyman Kontinuum Strahlung. Woher diese stammt ist bis heute eine offene Frage. In der vorliegenden Arbeit diskutiere ich die wahrscheinlichsten Kandidaten für die Emission dieser ionisierenden Strahlung: die Lyman alpha Emitter (LAE), eine Gruppe von Galaxien die man im frühen Universum antrifft. Hat nämlich ein Lyman Kontinuum Photon ein Wasserstoffatom ionisiert, kommt es häufig vor, dass sich Proton und Elektron wieder zu einem neutralen Wasserstoffatom verbinden. Bei diesem Prozess wird dann ein Lyman alpha Photon freigesetzt, was den LAE ihren Namen gibt. Da wir in den Spektren dieser Galaxien die Lyman alpha Photonen beobachten können, deren Voraussetzung die Existenz von Lyman Kontinuum Emission in der Galaxie ist, liegt es nahe anzunehmen, dass die Lyman Kontinuum Emission auch in das intergalaktische Medium vordringen kann um den Wasserstoff dort ebenfalls zu ionisieren. Durch diesen Mechanismus sind Lyman alpha und Lyman-Kontinuumsstrahlung eng miteinander verbunden und werden in dieser Arbeit beide untersucht, um die Eigenschaften von Galaxien im frühen Universum und den Zustand des Wasserstoffs im intergalaktischen Medium besser zu verstehen. Der erste Schritt ist jedoch die Detektion und korrekte Klassifizierung von LAE. Dafür benutze ich Daten des Multi-Unit Spectroscopic Explorer (MUSE), ein Instrument mit dem Beobachtungen möglich sind, die zwei räumliche Dimensionen mit einer spektralen Dimension verbinden. Somit ist in jedem Pixel der Daten ein Spektrum zur Verfügung, in dem nach Emissionslinien gesucht werden kann. Nach der Detektion von Emissionslinien in den MUSE-Daten wird die Aufgabe der Klassifizierung von der grafischen Benutzeroberfläche QtClassify unterstützt, die ich in dieser Arbeit entwickelt habe. Sie bietet dem Benutzer eine schnelle und übersichtliche Identifizierung der gefundenen Emissionslinien, was einen entscheidenden ersten Schritt zur Analyse der Eigenschaften der LAE darstellt. Da Lyman alpha Photonen in neutralem Wasserstoff, der im Inneren von Galaxien in Gaswolken vorkommt, gestreut wird, verändert sich die Form der Lyman alpha Emissionslinie im Spektrum. Nachdem also die LAE mit Hilfe von QtClassify identifiziert werden konnten, analysiere ich die Lyman alpha Linie hinsichtlich ihrer Breite, ihrer Symmetrie und ihrer Stärke und suche nach Doppellinien, die Hinweise auf die Kinematik der Wasserstoff Gaswolken geben. Besonders wichtig dabei ist die Stärke der Linie im Vergleich zum restlichen Spektrum, die sogenannte Äquivalentbreite. Dabei zeige ich, dass die übliche Methode die Verteilung der Äquivalentbreiten als Histogramme darzustellen ohne die Detektionsgrenzen der Beobachtungen miteinzubeziehen keine Aussage über die Eigenschaften der LAE, sondern lediglich über die Grenzen der Beobachtungen treffen. Daher konstruiere ich eine unabhängigere Verteilungsfunktion, die diese Grenzen mit einbezieht. Ich verdeutliche dies durch einen Vergleich des Anteils von Objekten mit hoher Äquivalentbreite in zwei verschiedenen Datensätzen, die auf Beobachtungen mit unterschiedlicher Belichtungszeit beruhen. Dabei finde ich in dem Datensatz mit der kürzeren Belichtungszeit einen Anteil von ~20% an Objekten mit hohen Äquivalentbreiten (über >240A) und nur ~1% im Datensatz mit der zehnfach längeren Belichtungszeit obwohl die Eigenschaften der LAE gleich sind. Zudem finde ich eine Galaxie mit einer Äquivalentbreite der Lyman alpha Linie von 600 +- 110A, was auf eine ungewöhnliche Sternpopulation hindeutet. Als letzten Schritt suche ich in den klassifizierten LAE nach Lyman Kontinuum, was für die Ionisierung des Wasserstoffs im intergalaktischen Medium verantwortlich ist, und untersuche den Zusammenhang zwischen der Lyman alpha und der Lyman Kontinuumsstrahlung. Um das Lyman Kontinuum detektieren zu können benutze ich Daten des Hubble-Weltraumteleskops (HST) und finde sechs Lyman Kontinuum Kandidaten unter den LAE. Um zu testen ob die Lyman Kontinuumsstrahlung lediglich von diesen Objekten ausgeht oder auch im der Gesamtheit der LAE zu finden ist, addiere ich die Daten des HST und finde ein Signal, was darauf hindeutet, dass ~80% der Lyman Kontinuumsstrahlung aus den Galaxien entkommen und in das intergalaktische Medium vordringen kann. Wenn das gefundene Signal zuverlässig ist deutet es darauf hin, dass in der Tat LAE für die Ionisierung des Wasserstoffs im Universum verantwortlich sein könnten. KW - astronomy KW - LAEs KW - reionization KW - Lyman alpha KW - Lyman continuum KW - VLT/MUSE KW - emission line classification KW - QtClassify KW - LAEs KW - Lyman alpha KW - Lyman Kontinuum KW - QtClassify KW - VLT/MUSE KW - Astronomie KW - Emissionslinienklassifikation KW - Reionisierung Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-478816 ER - TY - JOUR A1 - Vojta, Thomas A1 - Skinner, Sarah A1 - Metzler, Ralf T1 - Probability density of the fractional Langevin equation with reflecting walls JF - Physical review : E, Statistical, nonlinear and soft matter physics N2 - We investigate anomalous diffusion processes governed by the fractional Langevin equation and confined to a finite or semi-infinite interval by reflecting potential barriers. As the random and damping forces in the fractional Langevin equation fulfill the appropriate fluctuation-dissipation relation, the probability density on a finite interval converges for long times towards the expected uniform distribution prescribed by thermal equilibrium. In contrast, on a semi-infinite interval with a reflecting wall at the origin, the probability density shows pronounced deviations from the Gaussian behavior observed for normal diffusion. If the correlations of the random force are persistent (positive), particles accumulate at the reflecting wall while antipersistent (negative) correlations lead to a depletion of particles near the wall. We compare and contrast these results with the strong accumulation and depletion effects recently observed for nonthermal fractional Brownian motion with reflecting walls, and we discuss broader implications. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevE.100.042142 SN - 2470-0045 SN - 2470-0053 VL - 100 IS - 4 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Goychuk, Igor T1 - Fractional Hydrodynamic Memory and Superdiffusion in Tilted Washboard Potentials JF - Physical review letters N2 - Diffusion in tilted washboard potentials can paradoxically exceed free normal diffusion. The effect becomes much stronger in the underdamped case due to inertial effects. What happens upon inclusion of usually neglected fractional hydrodynamics memory effects (Basset-Boussinesq frictional force), which result in a heavy algebraic tail of the velocity autocorrelation function of the potential-free diffusion making it transiently superdiffusive? Will a giant enhancement of diffusion become even stronger, and the transient superdiffusion last even longer? These are the questions that we answer in this Letter based on an accurate numerical investigation. We show that a resonancelike enhancement of normal diffusion becomes indeed much stronger and sharper. Moreover, a long-lasting transient regime of superdiffusion, including Richardson-like diffusion, proportional to t(3) and ballistic supertransport, proportional to t(2), is revealed. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevLett.123.180603 SN - 0031-9007 SN - 1079-7114 VL - 123 IS - 18 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Haene, Janick A1 - Bruehwiler, Dominik A1 - Ecker, Achim A1 - Hass, Roland T1 - Real-time inline monitoring of zeolite synthesis by Photon Density Wave spectroscopy JF - Microporous and mesoporous materials : zeolites, clays, carbons and related materials N2 - The formation process of zeolite A (Linde Type A) was monitored inline at 1.5 L scale by Photon Density Wave (PDW) spectroscopy as novel process analytical technology for highly turbid liquid suspensions. As a result, the reduced scattering coefficient, being a measure for particle number, size, and morphology, provides distinct process information, including the formation of amorphous particles and their transfer into crystalline zeolite structures. The onset and end of the crystallization process can be detected inline and in real-time. Analyses by powder X-ray diffraction and electron microscopy, based on a sampling approach, support the interpretation of the results obtained by PDW spectroscopy. In addition, the influence of the molar water content was investigated, indicating a linear increase of the time needed to reach the end of the zeolite A crystallization with increasing molar water content. Further experiments indicate a strong influence of the silica source on the course of the crystallization. The applicability of PDW spectroscopy under even more demanding chemical and physical conditions was investigated by monitoring the synthesis of zeolite L (Linde Type L). KW - Photon density wave spectroscopy KW - Process analytical technology KW - Zeolite synthesis KW - Molar water content KW - Silica source Y1 - 2019 U6 - https://doi.org/10.1016/j.micromeso.2019.109580 SN - 1387-1811 SN - 1873-3093 VL - 288 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Jelken, Joachim A1 - Henkel, Carsten A1 - Santer, Svetlana T1 - Solving an old puzzle: fine structure of diffraction spots from an azo-polymer surface relief grating JF - Applied physics : B, Lasers and optics N2 - We report on the experimental and theoretical interpretation of the diffraction of a probe beam during inscription of a surface relief grating with an interference pattern into a photo-responsive polymer film. For this, we developed a set-up allowing for the simultaneous recording of the diffraction efficiency (DE), the fine structure of the diffraction spot and the topographical changes, in situ and in real time while the film is irradiated. The time dependence of the DE, as the surface relief deepens, follows a Bessel function exhibiting maxima and minima. The size of the probe beam relative to the inscribed grating (i.e., to the size of the writing beams) matters and has to be considered for the interpretation of the DE signal. It is also at the origin of a fine structure within the diffraction spot where ring-shaped features appear once an irradiation time corresponding to the first maximum of the DE has been exceeded. Y1 - 2019 U6 - https://doi.org/10.1007/s00340-019-7331-8 SN - 0946-2171 SN - 1432-0649 VL - 125 IS - 11 PB - Springer CY - Heidelberg ER - TY - JOUR A1 - Metzler, Ralf T1 - Brownian motion and beyond: first-passage, power spectrum, non-Gaussianity, and anomalous diffusion JF - Journal of statistical mechanics: theory and experiment N2 - Brownian motion is a ubiquitous physical phenomenon across the sciences. After its discovery by Brown and intensive study since the first half of the 20th century, many different aspects of Brownian motion and stochastic processes in general have been addressed in Statistical Physics. In particular, there now exists a very large range of applications of stochastic processes in various disciplines. Here we provide a summary of some of the recent developments in the field of stochastic processes, highlighting both the experimental findings and theoretical frameworks. KW - 15 KW - 4 Y1 - 2019 U6 - https://doi.org/10.1088/1742-5468/ab4988 SN - 1742-5468 VL - 2019 IS - 11 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Bohdan, Artem A1 - Niemiec, Jacek A1 - Pohl, Martin A1 - Matsumoto, Yosuke A1 - Amano, Takanobu A1 - Hoshino, Masahiro T1 - Kinetic Simulations of Nonrelativistic Perpendicular Shocks of Young Supernova Remnants. II. Influence of Shock-surfing Acceleration on Downstream Electron Spectra JF - The astrophysical journal : an international review of spectroscopy and astronomical physics N2 - We explore electron preacceleration at high-Mach-number nonrelativistic perpendicular shocks at, e.g., young supernova remnants, which are a prerequisite of further acceleration to very high energies via diffusive shock acceleration. Using fully kinetic particle-in-cell simulations of shocks and electron dynamics in them, we investigate the influence of shock-surfing acceleration (SSA) at the shock foot on the nonthermal population of electrons downstream of the shock. The SSA is followed by further energization at the shock ramp where the Weibel instability spawns a type of second-order Fermi acceleration. The combination of these two processes leads to the formation of a nonthermal electron population, but the importance of SSA becomes smaller for larger ion-to-electron mass ratios in the simulation. We discuss the resulting electron spectra and the relevance of our results to the physics of systems with real ion-to-electron mass ratios and fully three-dimensional behavior. KW - Shocks KW - Space plasmas KW - Supernova remnants KW - Interstellar medium Y1 - 2019 U6 - https://doi.org/10.3847/1538-4357/ab43cf SN - 0004-637X SN - 1538-4357 VL - 885 IS - 1 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Plat, A. A1 - Charlot, S. A1 - Bruzual, G. A1 - Feltre, A. A1 - Vidal-Garcia, A. A1 - Morisset, C. A1 - Chevallard, Jacopo A1 - Todt, Helge Tobias T1 - Constraints on the production and escape of ionizing radiation from the emission-line spectra of metal-poor star-forming galaxies JF - Monthly notices of the Royal Astronomical Society N2 - We explore the production and escape of ionizing photons in young galaxies by investigating the ultraviolet and optical emission-line properties of models of ionization-bounded and density-bounded H II regions, active-galactic-nucleus (AGN) narrow-line regions, and radiative shocks computed all using the same physically consistent description of element abundances and depletion on to dust grains down to very low metallicities. We compare these models with a reference sample of metal-poor star-forming galaxies and Lyman-continuum (LyC) leakers at various redshifts, which allows the simultaneous exploration of more spectral diagnostics than typically available at once for individual subsamples. We confirm that current single- and binary-star population synthesis models do not produce hard-enough radiation to account for the high-ionization emission of the most metal-poor galaxies. Introducing either an AGN or radiative-shock component brings models into agreement with observations. A published model including X-ray binaries is an attractive alternative to reproduce the observed rise in He II lambda 4686/H beta ratio with decreasing oxygen abundance in metal-poor star-forming galaxies, but not the high observed He II lambda 4686/H beta ratios of galaxies with large EW(H beta). A source of harder ionizing radiation appears to be required in these extreme objects, such as an AGN or radiative-shock component, perhaps linked to an initial-mass-function bias towards massive stars at low metallicity. This would also account for the surprisingly high [O I]/[O III] ratios of confirmed LyC leakers relative to ionization-bounded models. We find no simple by-eye diagnostic of the nature of ionizing sources and the escape of LyC photon, which require proper simultaneous fits of several lines to be discriminated against. KW - galaxies: general KW - galaxies: high-redshift KW - galaxies: ISM Y1 - 2019 U6 - https://doi.org/10.1093/mnras/stz2616 SN - 0035-8711 SN - 1365-2966 VL - 490 IS - 1 SP - 978 EP - 1009 PB - Oxford Univ. Press CY - Oxford ER - TY - JOUR A1 - Diercke, Andrea A1 - Denker, Carsten T1 - Chromospheric Synoptic Maps of Polar Crown Filaments JF - Solar physics : a journal for solar and solar-stellar research and the study of solar terrestrial physics N2 - Polar crown filaments form above the polarity inversion line between the old magnetic flux of the previous cycle and the new magnetic flux of the current cycle. Studying their appearance and their properties can lead to a better understanding of the solar cycle. We use full-disk data of the Chromospheric Telescope (ChroTel) at the Observatorio del Teide, Tenerife, Spain, which were taken in three different chromospheric absorption lines (H alpha lambda 6563 angstrom, Ca II K lambda 3933 angstrom, and He I lambda 10830 angstrom), and we create synoptic maps. In addition, the spectroscopic He I data allow us to compute Doppler velocities and to create synoptic Doppler maps. ChroTel data cover the rising and decaying phase of Solar Cycle 24 on about 1000 days between 2012 and 2018. Based on these data, we automatically extract polar crown filaments with image-processing tools and study their properties. We compare contrast maps of polar crown filaments with those of quiet-Sun filaments. Furthermore, we present a super-synoptic map summarizing the entire ChroTel database. In summary, we provide statistical properties, i.e. number and location of filaments, area, and tilt angle for both the maximum and the declining phase of Solar Cycle 24. This demonstrates that ChroTel provides a promising data set to study the solar cycle. KW - Chromosphere, quiet KW - Prominences, quiescent KW - Prominences, magnetic field KW - Solar Cycle, observations KW - Instrumentation and data management Y1 - 0201 U6 - https://doi.org/10.1007/s11207-019-1538-z SN - 0038-0938 SN - 1573-093X VL - 294 IS - 11 PB - Springer CY - Dordrecht ER - TY - JOUR A1 - Drozdov, Alexander A1 - Aseev, Nikita A1 - Effenberger, Frederic A1 - Turner, Drew L. A1 - Saikin, Anthony A1 - Shprits, Yuri Y. T1 - Storm Time Depletions of Multi-MeV Radiation Belt Electrons Observed at Different Pitch Angles JF - Journal of geophysical research : Space physics N2 - During geomagnetic storms, the rapid depletion of the high-energy (several MeV) outer radiation belt electrons is the result of loss to the interplanetary medium through the magnetopause, outward radial diffusion, and loss to the atmosphere due to wave-particle interactions. We have performed a statistical study of 110 storms using pitch angle resolved electron flux measurements from the Van Allen Probes mission and found that inside of the radiation belt (L* = 3 - 5) the number of storms that result in depletion of electrons with equatorial pitch angle alpha(eq) = 30 degrees is higher than number of storms that result in depletion of electrons with equatorial pitch angle alpha(eq) = 75 degrees. We conclude that this result is consistent with electron scattering by whistler and electromagnetic ion cyclotron waves. At the outer edge of the radiation belt (L* >= 5.2) the number of storms that result in depletion is also large (similar to 40-50%), emphasizing the significance of the magnetopause shadowing effect and outward radial transport. Y1 - 2019 U6 - https://doi.org/10.1029/2019JA027332 SN - 2169-9380 SN - 2169-9402 VL - 124 IS - 11 SP - 8943 EP - 8953 PB - American Geophysical Union CY - Washington ER - TY - JOUR A1 - Teomy, Eial A1 - Roichman, Yael A1 - Shokef, Yair T1 - Multiple peaks in the displacement distribution of active random walkers JF - Journal of statistical mechanics: theory and experiment N2 - We consider a simple model for active random walk with general temporal correlations, and investigate the shape of the probability distribution function of the displacement during a short time interval. We find that under certain conditions the distribution exhibits multiple peaks and we show analytically and numerically that the existence of these peaks is governed by the walker?s tendency to move forward, while the correlations between the timing of its active motion control the magnitude and shape of the peaks. In particular, we find that in a homogeneous system such peaks can occur only if the persistence is strong enough. KW - 16 KW - 4 Y1 - 2019 U6 - https://doi.org/10.1088/1742-5468/ab4fde SN - 1742-5468 VL - 2019 IS - 11 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Powierza, Bartosz A1 - Gollwitzer, Christian A1 - Wolgast, Dagmar A1 - Staude, Andreas A1 - Bruno, Giovanni T1 - Fully experiment-based evaluation of few digital volume correlation techniques JF - Review of scientific instruments : a monthly journal devoted to scientific instruments, apparatus, and techniques N2 - Digital Volume Correlation (DVC) is a powerful set of techniques used to compute the local shifts of 3D images obtained, for instance, in tomographic experiments. It is utilized to analyze the geometric changes of the investigated object as well as to correct the corresponding image misalignments for further analysis. It can therefore be used to evaluate the local density changes of the same regions of the inspected specimens, which might be shifted between measurements. In recent years, various approaches and corresponding pieces of software were introduced. Accuracies for the computed shift vectors of up to about 1 parts per thousand of a single voxel size have been reported. These results, however, were based either on synthetic datasets or on an unrealistic setup. In this work, we propose two simple methods to evaluate the accuracy of DVC-techniques using more realistic input data and apply them to several DVC programs. We test these methods on three materials (tuff, sandstone, and concrete) that show different contrast and structural features. Published under license by AIP Publishing. Y1 - 2019 U6 - https://doi.org/10.1063/1.5099572 SN - 0034-6748 SN - 1089-7623 VL - 90 IS - 11 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Bolotov, Dmitry A1 - Bolotov, Maxim I. A1 - Smirnov, Lev A. A1 - Osipov, Grigory V. A1 - Pikovskij, Arkadij T1 - Twisted States in a System of Nonlinearly Coupled Phase Oscillators JF - Regular and chaotic dynamics : international scientific journal N2 - We study the dynamics of the ring of identical phase oscillators with nonlinear nonlocal coupling. Using the Ott - Antonsen approach, the problem is formulated as a system of partial derivative equations for the local complex order parameter. In this framework, we investigate the existence and stability of twisted states. Both fully coherent and partially coherent stable twisted states were found (the latter ones for the first time for identical oscillators). We show that twisted states can be stable starting from a certain critical value of the medium length, or on a length segment. The analytical results are confirmed with direct numerical simulations in finite ensembles. KW - twisted state KW - phase oscillators KW - nonlocal coupling KW - Ott - Antonsen reduction KW - stability analysis Y1 - 2019 U6 - https://doi.org/10.1134/S1560354719060091 SN - 1560-3547 SN - 1468-4845 VL - 24 IS - 6 SP - 717 EP - 724 PB - Pleiades publishing inc CY - Moscow ER - TY - JOUR A1 - Hsu, H. F. A1 - Krekhov, Andrey A1 - Tarantola, Marco A1 - Beta, Carsten A1 - Bodenschatz, Eberhardt T1 - Interplay between myosin II and actin dynamics in chemotactic amoeba JF - New journal of physics : the open-access journal for physics N2 - The actin cytoskeleton and its response to external chemical stimuli is fundamental to the mechano-biology of eukaryotic cells and their functions. One of the key players that governs the dynamics of the actin network is the motor protein myosin II. Based on a phase space embedding we have identified from experiments three phases in the cytoskeletal dynamics of starved Dictyostelium discoideum in response to a precisely controlled chemotactic stimulation. In the first two phases the dynamics of actin and myosin II in the cortex is uncoupled, while in the third phase the time scale for the recovery of cortical actin is determined by the myosin II dynamics. We report a theoretical model that captures the experimental observations quantitatively. The model predicts an increase in the optimal response time of actin with decreasing myosin II-actin coupling strength highlighting the role of myosin II in the robust control of cell contraction. KW - actin KW - myosin II KW - chemotaxis KW - oscillations KW - coupling KW - delay differential equation KW - contraction Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab5822 SN - 1367-2630 VL - 21 IS - 11 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Göttgens, Fabian A1 - Husser, Tim-Oliver A1 - Kamann, Sebastian A1 - Dreizler, Stefan A1 - Giesers, Benjamin A1 - Kollatschny, Wolfram A1 - Weilbacher, Peter Michael A1 - Roth, Martin M. A1 - Wendt, Martin T1 - A stellar census in globular clusters with MUSE: A spectral catalogue of emission-line sources JF - Astronomy and astrophysics : an international weekly journal N2 - Aims. Globular clusters produce many exotic stars due to a much higher frequency of dynamical interactions in their dense stellar environments. Some of these objects were observed together with several hundred thousand other stars in our MUSE survey of 26 Galactic globular clusters. Assuming that at least a few exotic stars have exotic spectra (i.e. spectra that contain emission lines), we can use this large spectroscopic data set of over a million stellar spectra as a blind survey to detect stellar exotica in globular clusters. Methods. To detect emission lines in each spectrum, we modelled the expected shape of an emission line as a Gaussian curve. This template was used for matched filtering on the di fferences between each observed 1D spectrum and its fitted spectral model. The spectra with the most significant detections of H alpha emission are checked visually and cross-matched with published catalogues. Results. We find 156 stars with H alpha emission, including several known cataclysmic variables (CV) and two new CVs, pulsating variable stars, eclipsing binary stars, the optical counterpart of a known black hole, several probable sub-subgiants and red stragglers, and 21 background emission-line galaxies. We find possible optical counterparts to 39 X-ray sources, as we detected H alpha emission in several spectra of stars that are close to known positions of Chandra X-ray sources. This spectral catalogue can be used to supplement existing or future X-ray or radio observations with spectra of potential optical counterparts to classify the sources. KW - globular clusters: general KW - stars: emission-line, Be KW - novae KW - cataclysmic variables KW - catalogs KW - techniques: imaging spectroscopy Y1 - 2019 U6 - https://doi.org/10.1051/0004-6361/201936485 SN - 0004-6361 SN - 1432-0746 VL - 631 PB - EDP Sciences CY - Les Ulis ER - TY - JOUR A1 - Padash, Amin A1 - Chechkin, Aleksei V. A1 - Dybiec, Bartlomiej A1 - Pavlyukevich, Ilya A1 - Shokri, Babak A1 - Metzler, Ralf T1 - First-passage properties of asymmetric Levy flights JF - Journal of physics : A, Mathematical and theoretical N2 - Lévy flights are paradigmatic generalised random walk processes, in which the independent stationary increments—the 'jump lengths'—are drawn from an -stable jump length distribution with long-tailed, power-law asymptote. As a result, the variance of Lévy flights diverges and the trajectory is characterised by occasional extremely long jumps. Such long jumps significantly decrease the probability to revisit previous points of visitation, rendering Lévy flights efficient search processes in one and two dimensions. To further quantify their precise property as random search strategies we here study the first-passage time properties of Lévy flights in one-dimensional semi-infinite and bounded domains for symmetric and asymmetric jump length distributions. To obtain the full probability density function of first-passage times for these cases we employ two complementary methods. One approach is based on the space-fractional diffusion equation for the probability density function, from which the survival probability is obtained for different values of the stable index and the skewness (asymmetry) parameter . The other approach is based on the stochastic Langevin equation with -stable driving noise. Both methods have their advantages and disadvantages for explicit calculations and numerical evaluation, and the complementary approach involving both methods will be profitable for concrete applications. We also make use of the Skorokhod theorem for processes with independent increments and demonstrate that the numerical results are in good agreement with the analytical expressions for the probability density function of the first-passage times. KW - Levy flights KW - first-passage KW - search dynamics Y1 - 2019 U6 - https://doi.org/10.1088/1751-8121/ab493e SN - 1751-8113 SN - 1751-8121 VL - 52 IS - 45 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Maheswaran, Rathinasamy A1 - Agarwal, Ankit A1 - Sivakumar, Bellie A1 - Marwan, Norbert A1 - Kurths, Jürgen T1 - Wavelet analysis of precipitation extremes over India and teleconnections to climate indices JF - Stochastic Environmental Research and Risk Assessment N2 - Precipitation patterns and extremes are significantly influenced by various climatic factors and large-scale atmospheric circulation patterns. This study uses wavelet coherence analysis to detect significant interannual and interdecadal oscillations in monthly precipitation extremes across India and their teleconnections to three prominent climate indices, namely, Nino 3.4, Pacific Decadal Oscillation, and Indian Ocean Dipole (IOD). Further, partial wavelet coherence analysis is used to estimate the standalone relationship between the climate indices and precipitation after removing the effect of interdependency. The wavelet analysis of monthly precipitation extremes at 30 different locations across India reveals that (a) interannual (2-8 years) and interdecadal (8-32 years) oscillations are statistically significant, and (b) the oscillations vary in both time and space. The results from the partial wavelet coherence analysis reveal that Nino 3.4 and IOD are the significant drivers of Indian precipitation at interannual and interdecadal scales. Intriguingly, the study also confirms that the strength of influence of large-scale atmospheric circulation patterns on Indian precipitation extremes varies with spatial physiography of the region. KW - Extreme precipitation KW - Teleconnection patterns KW - Wavelets KW - Partial wavelet coherence KW - India Y1 - 2019 U6 - https://doi.org/10.1007/s00477-019-01738-3 SN - 1436-3240 SN - 1436-3259 VL - 33 IS - 11-12 SP - 2053 EP - 2069 PB - Springer CY - New York ER - TY - JOUR A1 - Le Quang Phuong, A1 - Hosseini, Seyed Mehrdad A1 - Koh, Chang Woo A1 - Woo, Han Young A1 - Shoaee, Safa T1 - Measuring Competing Recombination Losses in a Significantly Reduced Langevin System by Steady-State Photoinduced Absorption and Photocurrent Spectroscopy JF - The journal of physical chemistry : C, Nanomaterials and interfaces N2 - Understanding and disentangling photophysical properties of long-lived photoexcitations in bulk heterojunction (BHJ) solar cells, which contribute mostly to photocurrent, provide essential guidelines to their improvement. However, to construct improved physical models, their rational design relies on reliable measurement techniques for charge recombination. Here, we combine photocurrent and photoinduced absorption spectroscopy (PCPIA) to directly probe the free carrier concentration and investigate loss mechanisms of long-lived excitations in nearly 10% efficient PPDT2FBT/PC70BM BHJ solar cells under steady-state operational conditions. From the PCPIA data obtained under open- circuit and short-circuit conditions, the absorption cross section and the concentration of photoexcitations are obtained. This material system exhibits an exceptionally low bimolecular recombination rate, about 300 times smaller than the diffusion-controlled electron and hole encounter rate. Furthermore, we observe that the fill factor is limited by losses originating from long-lived photoexcitations undergoing dispersive bimolecular recombination. Y1 - 2019 U6 - https://doi.org/10.1021/acs.jpcc.9b08901 SN - 1932-7447 SN - 1932-7455 VL - 123 IS - 45 SP - 27417 EP - 27422 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Liu, Ji-Cai A1 - Vaz da Cruz, Vinicius A1 - Polyutov, Sergey A1 - Föhlisch, Alexander T1 - Recoil-induced dissociation in hard-x-ray photoionization JF - Physical review : A, Atomic, molecular, and optical physics N2 - We predict the recoil-induced molecular dissociation in hard-x-ray photoionization. The recoil effect is caused by electronic and photon momentum exchange with the molecule. We show the strong role of relativistic effects for the studied molecular fragmentation. The recoil-induced fragmentation of the molecule is caused by elongation of the bond due to the vibrational recoil effect and because of the centrifugal force caused by the rotational recoil. The calculations of the x-ray photoelectron spectra of the H-2 and NO molecules show that the predicted effects can be observed in high-energy synchrotrons like SOLEIL, SPring-8, PETRA, and XFEL SACLA. The relativistic effect enhances the recoil momentum transfer and makes it strongly sensitive to the direction of ejection of the fast photoelectron with respect to the photon momentum. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevA.100.053408 SN - 2469-9926 SN - 2469-9934 VL - 100 IS - 5 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Ueckerdt, Falko A1 - Frieler, Katja A1 - Lange, Stefan A1 - Wenz, Leonie A1 - Luderer, Gunnar A1 - Levermann, Anders T1 - The economically optimal warming limit of the planet JF - Earth system dynamics N2 - Both climate-change damages and climate-change mitigation will incur economic costs. While the risk of severe damages increases with the level of global warming (Dell et al., 2014; IPCC, 2014b, 2018; Lenton et al., 2008), mitigating costs increase steeply with more stringent warming limits (IPCC, 2014a; Luderer et al., 2013; Rogelj et al., 2015). Here, we show that the global warming limit that minimizes this century's total economic costs of climate change lies between 1.9 and 2 ∘C, if temperature changes continue to impact national economic growth rates as observed in the past and if instantaneous growth effects are neither compensated nor amplified by additional growth effects in the following years. The result is robust across a wide range of normative assumptions on the valuation of future welfare and inequality aversion. We combine estimates of climate-change impacts on economic growth for 186 countries (applying an empirical damage function from Burke et al., 2015) with mitigation costs derived from a state-of-the-art energy–economy–climate model with a wide range of highly resolved mitigation options (Kriegler et al., 2017; Luderer et al., 2013, 2015). Our purely economic assessment, even though it omits non-market damages, provides support for the international Paris Agreement on climate change. The political goal of limiting global warming to “well below 2 degrees” is thus also an economically optimal goal given above assumptions on adaptation and damage persistence. Y1 - 2019 U6 - https://doi.org/10.5194/esd-10-741-2019 SN - 2190-4979 SN - 2190-4987 VL - 10 IS - 4 SP - 741 EP - 763 PB - Copernicus CY - Göttingen ER - TY - JOUR A1 - Lever, Fabiano A1 - Ramelow, Sven A1 - Gühr, Markus T1 - Effects of time-energy correlation strength in molecular entangled photon spectroscopy JF - Physical review : A, Atomic, molecular, and optical physics N2 - In this paper, we explore the time-energy domain quantum-classical transition comparing a classical pump-probe experiment on a diatomic molecule to its quantum enhanced counterpart, where the pump and probe pulses are substituted by the signal and idler beams of a spontaneous parametric down conversion (SPDC) source. Absorption of biphotons generated with SPDC exploits quantum time-energy entanglement to enhance the overall yield and selectivity of the process, when compared with a classical pump-probe setup, while maintaining femtosecond time resolution. We systematically study the effects of correlation strength on process efficiency and selectivity, comparing the results to classical pump-probe spectra. An excitation scheme to improve the yield based on spectral narrowing of biphotons is shown. The results indicate that the quantum improvements in yield are caused by a more efficient use of the total power available for the process. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevA.100.053844 SN - 2469-9926 SN - 2469-9934 VL - 100 IS - 5 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Liu, Ruo-Yu A1 - Yan, Huirong A1 - Zhang, Heshou T1 - Role of Anisotropic Diffusion of Particles JF - Physical review letters N2 - In this Letter, we propose that the x-ray and the TeV observations in the vicinity of Geminga can be understood in the framework of anisotropic diffusion of injected electrons or positrons. This interpretation only requires the turbulence in the vicinity of Geminga to be sub-Alfvenic with the local mean magnetic field direction approximately aligned with our line of sight towards Geminga, without invoking extreme conditions for the environment, such as an extremely small diffusion coefficient and a weak magnetic field of submicrogauss as suggested in previous literature. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevLett.123.221103 SN - 0031-9007 SN - 1079-7114 VL - 123 IS - 22 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Kniepert, Juliane A1 - Paulke, Andreas A1 - Perdigón-Toro, Lorena A1 - Kurpiers, Jona A1 - Zhang, Huotian A1 - Gao, Feng A1 - Yuan, Jun A1 - Zou, Yingping A1 - Le Corre, Vincent M. A1 - Koster, Lambert Jan Anton A1 - Neher, Dieter T1 - Reliability of charge carrier recombination data determined with charge extraction methods JF - Journal of applied physics N2 - Charge extraction methods are popular for measuring the charge carrier density in thin film organic solar cells and to draw conclusions about the order and coefficient of nongeminate charge recombination. However, results from such studies may be falsified by inhomogeneous steady state carrier profiles or surface recombination. Here, we present a detailed drift-diffusion study of two charge extraction methods, bias-assisted charge extraction (BACE) and time-delayed collection field (TDCF). Simulations are performed over a wide range of the relevant parameters. Our simulations reveal that both charge extraction methods provide reliable information about the recombination order and coefficient if the measurements are performed under appropriate conditions. However, results from BACE measurements may be easily affected by surface recombination, in particular for small active layer thicknesses and low illumination densities. TDCF, on the other hand, is more robust against surface recombination due to its transient nature but also because it allows for a homogeneous high carrier density to be inserted into the active layer. Therefore, TDCF is capable to provide meaningful information on the order and coefficient of recombination even if the model conditions are not exactly fulfilled. We demonstrate this for an only 100 nm thick layer of a highly efficient nonfullerene acceptor (NFA) blend, comprising the donor polymer PM6 and the NFA Y6. TDCF measurements were performed as a function of delay time for different laser fluences and bias conditions. The full set of data could be consistently fitted by a strict second order recombination process, with a bias- and fluence-independent bimolecular recombination coefficient k(2) = 1.7 x 10(-17)m(3) s(-1). BACE measurements performed on the very same layer yielded the identical result, despite the very different excitation conditions. This proves that recombination in this blend is mostly through processes in the bulk and that surface recombination is of minor importance despite the small active layer thickness. Published under license by AIP Publishing. Y1 - 2019 U6 - https://doi.org/10.1063/1.5129037 SN - 0021-8979 SN - 1089-7550 VL - 126 IS - 20 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Patel, Dhananjay I. A1 - Noack, Sebastian A1 - Vacogne, Charlotte D. A1 - Schlaad, Helmut A1 - Bahr, Stephan A1 - Dietrich, Paul A1 - Meyer, Michael A1 - Thissen, Andreas A1 - Linford, Matthew R. T1 - Poly(L-lactic acid), by near-ambient pressure XPS JF - Surface Science Spectra N2 - Near ambient pressure - x-ray photoelectron spectroscopy (NAP-XPS) is a less traditional form of XPS that allows samples to be analyzed at relatively high pressures, i.e., at 2500Pa or higher. With NAP-XPS, one can analyze moderately volatile liquids, biological samples, porous materials, and/or polymeric materials that outgas significantly. In this submission we show C 1s, O 1s, and survey NAP-XPS spectra from poly(L-lactic acid). The C 1s and O 1s envelopes were fit with three and two Gaussian-Lorentzian sum functions, respectively. Water vapor (800Pa) was used as the residual gas for charge compensation, which was confirmed by the sharp peak at 535.0 eV in the O 1s narrow scan. The uniqueness plot corresponding to the C 1s fit shows that the fit parameters had statistical significance. C 1s and O 1s spectra of PLLA damaged by exposure to x-rays for ca. 1 hour are also included. Published by the AVS. KW - near-ambient pressure X-ray photoelectron spectroscopy KW - NAP-XPS KW - XPS KW - Water Vapor Y1 - 2019 U6 - https://doi.org/10.1116/1.5110309 SN - 1055-5269 SN - 1520-8575 VL - 26 IS - 2 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Gengel, Erik A1 - Pikovskij, Arkadij T1 - Phase demodulation with iterative Hilbert transform embeddings JF - Signal processing N2 - We propose an efficient method for demodulation of phase modulated signals via iterated Hilbert transform embeddings. We show that while a usual approach based on one application of the Hilbert transform provides only an approximation to a proper phase, with iterations the accuracy is essentially improved, up to precision limited mainly by discretization effects. We demonstrate that the method is applicable to arbitrarily complex waveforms, and to modulations fast compared to the basic frequency. Furthermore, we develop a perturbative theory applicable to a simple cosine waveform, showing convergence of the technique. KW - Phase modulation KW - Hilbert transform KW - Embedding Y1 - 2019 U6 - https://doi.org/10.1016/j.sigpro.2019.07.005 SN - 0165-1684 SN - 1872-7557 VL - 165 SP - 115 EP - 127 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Raman Venkatesan, Thulasinath A1 - Gulyakova, Anna A. A1 - Frübing, Peter A1 - Gerhard, Reimund T1 - Electrical polarization phenomena, dielectric relaxations and structural transitions in a relaxor-ferroelectric terpolymer investigated with electrical probing techniques JF - Materials research express N2 - Dielectric Relaxation Spectroscopy (DRS) and Thermally Stimulated Depolarization Current (TSDC) measurements were employed to study dielectric-relaxation processes, structural transitions and electric-polarization phenomena in poly(vinylidenefluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)) terpolymer films. Results from DRS confirm the existence of two separate dispersion regions related to a para-to-ferroelectric phase transition and to the glass transition. The dipolar TSDC peak correlates with the loss peak of the ? relaxation that represents the glass transition. The electric polarization calculated from the dipolar TSDC peak (glass transition) shows a non-linear electric-field dependence and saturates at high electric poling fields. As the observed behaviour is essentially the same as that of the electric polarization obtained from direct polarization-versus-electric-field hysteresis measurements, TSDC experiments are also suitable for studying the polarization in relaxor-ferroelectric polymers. A saturation polarization of 44 mC m(?2) was found for an electric field of 190 MV m(?1). KW - P(VDF-TrFE-CFE) terpolymer KW - relaxor-ferroelectric polymers KW - dielectric relaxation spectroscopy KW - thermally stimulated depolarization current KW - electrical polarization hysteresis Y1 - 2019 U6 - https://doi.org/10.1088/2053-1591/ab5352 SN - 2053-1591 VL - 6 IS - 12 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Rüdiger, Günther A1 - Schultz, M. T1 - Non-diffusive angular momentum transport in rotating z-pinches JF - Journal of plasma physics N2 - The stability of conducting Taylor-Couette flows under the presence of toroidal magnetic background fields is considered. For strong enough magnetic amplitudes such magnetohydrodynamic flows are unstable against non-axisymmetric perturbations which may also transport angular momentum. In accordance with the often used diffusion approximation, one expects the angular momentum transport to be vanishing for rigid rotation. In the sense of a non-diffusive Lambda effect, however, even for rigidly rotating z-pinches, an axisymmetric angular momentum flux appears which is directed outward (inward) for large (small) magnetic Mach numbers. The internal rotation in a magnetized rotating tank can thus never be uniform. Those particular rotation laws are used to estimate the value of the instability-induced eddy viscosity for which the non-diffusive Lambda effect and the diffusive shear-induced transport compensate each other. The results provide the Shakura & Sunyaev viscosity ansatz leading to numerical values linearly growing with the applied magnetic field. KW - plasma instabilities KW - astrophysical plasmas Y1 - 2019 U6 - https://doi.org/10.1017/S0022377819000606 SN - 0022-3778 SN - 1469-7807 VL - 85 IS - 6 PB - Cambridge Univ. Press CY - New York ER - TY - JOUR A1 - Berrah, N. A1 - Sánchez-González, Álvaro A1 - Jurek, Zoltan A1 - Obaid, Razib A1 - Xiong, H. A1 - Squibb, R. J. A1 - Osipov, T. A1 - Lutman, A. A1 - Fang, L. A1 - Barillot, T. A1 - Bozek, J. D. A1 - Cryan, J. A1 - Wolf, T. J. A. A1 - Rolles, Daniel A1 - Coffee, R. A1 - Schnorr, Kirsten A1 - Augustin, S. A1 - Fukuzawa, Hironobu A1 - Motomura, K. A1 - Niebuhr, Nina Isabelle A1 - Frasinski, L. J. A1 - Feifel, Raimund A1 - Schulz, Claus-Peter A1 - Toyota, Kenji A1 - Son, Sang-Kil A1 - Ueda, K. A1 - Pfeifer, T. A1 - Marangos, J. P. A1 - Santra, Robin T1 - Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization JF - Nature physics N2 - X-ray free-electron lasers have, over the past decade, opened up the possibility of understanding the ultrafast response of matter to intense X-ray pulses. In earlier research on atoms and small molecules, new aspects of this response were uncovered, such as rapid sequences of inner-shell photoionization and Auger ionization. Here, we studied a larger molecule, buckminsterfullerene (C-60), exposed to 640 eV X-rays, and examined the role of chemical effects, such as chemical bonds and charge transfer, on the fragmentation following multiple ionization of the molecule. To provide time resolution, we performed femtosecond-resolved X-ray pump/X-ray probe measurements, which were accompanied by advanced simulations. The simulations and experiment reveal that despite substantial ionization induced by the ultrashort (20 fs) X-ray pump pulse, the fragmentation of C-60 is considerably delayed. This work uncovers the persistence of the molecular structure of C-60, which hinders fragmentation over a timescale of hundreds of femtoseconds. Furthermore, we demonstrate that a substantial fraction of the ejected fragments are neutral carbon atoms. These findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules. Y1 - 2019 U6 - https://doi.org/10.1038/s41567-019-0665-7 SN - 1745-2473 SN - 1745-2481 VL - 15 IS - 12 SP - 1279 EP - 1301 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Stolterfoht, Martin A1 - Le Corre, Vincent M. A1 - Feuerstein, Markus A1 - Caprioglio, Pietro A1 - Koster, Lambert Jan Anton A1 - Neher, Dieter T1 - Voltage-Dependent Photoluminescence and How It Correlates with the Fill Factor and Open-Circuit Voltage in Perovskite Solar Cells JF - Acs energy letters N2 - Optimizing the photoluminescence (PL) yield of a solar cell has long been recognized as a key principle to maximize the power conversion efficiency. While PL measurements are routinely applied to perovskite films and solar cells under open circuit conditions (V-OC), it remains unclear how the emission depends on the applied voltage. Here, we performed PL(V) measurements on perovskite cells with different hole transport layer thicknesses and doping concentrations, resulting in remarkably different fill factors (FFs). The results reveal that PL(V) mirrors the current-voltage (JV) characteristics in the power-generating regime, which highlights an interesting correlation between radiative and nonradiative recombination losses. In particular, high FF devices show a rapid quenching of PL(V) from open-circuit to the maximum power point. We conclude that, while the PL has to be maximized at V-OC at lower biases < V-OC the PL must be rapidly quenched as charges need to be extracted prior to recombination. Y1 - 2019 U6 - https://doi.org/10.1021/acsenergylett.9b02262 SN - 2380-8195 VL - 4 IS - 12 SP - 2887 EP - 2892 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Schroetter, Ilane A1 - Bouche, Nicolas F. A1 - Zabl, Johannes A1 - Contini, Thierry A1 - Wendt, Martin A1 - Schaye, Joop A1 - Mitchell, Peter A1 - Muzahid, Sowgat A1 - Marino, Raffaella Anna A1 - Bacon, Roland A1 - Lilly, Simon J. A1 - Richard, Johan A1 - Wisotzki, Lutz T1 - MusE GAs FLOw andWind (MEGAFLOW) BT - III. Galactic wind properties using background quasars JF - Monthly notices of the Royal Astronomical Society N2 - We present results from our on-going MusE GAs FLOw and Wind (MEGAFLOW) survey, which consists of 22 quasar lines of sight, each observed with the integral field unit MUSE and the UVES spectrograph at the ESO Very Large Telescopes (VLT). The goals of this survey are to study the properties of the circumgalactic medium around z similar to 1 star-forming galaxies. The absorption-line selected survey consists of 79 strong MgII absorbers (with rest-frame equivalent width greater than or similar to 0.3 angstrom) and, currently, 86 associated galaxies within 100 projected kpc of the quasar with stellar masses (M-star) from 109 to 1011 M-circle dot. We find that the cool halo gas traced by MgII is not isotropically distributed around these galaxies from the strong bi-modal distribution in the azimuthal angle of the apparent location of the quasar with respect to the galaxy major axis. This supports a scenario in which outflows are bi-conical in nature and co-exist with a co-planar gaseous structure extending at least up to 60-80 kpc. Assuming that absorbers near the minor axis probe outflows, the current MEGAFLOW sample allowed us to select 26 galaxy-quasar pairs suitable for studying winds. From this sample, using a simple geometrical model, we find that the outflow velocity only exceeds the escape velocity when M-star less than or similar to 4 x 10(9) M-circle dot, implying the cool material is likely to fall back except in the smallest haloes. Finally, we find that the mass loading factor., the ratio between the ejected mass rate and the star formation rate, appears to be roughly constant with respect to the galaxy mass. KW - galaxies: evolution KW - galaxies: formation KW - intergalactic medium KW - quasars: absorption lines Y1 - 2019 U6 - https://doi.org/10.1093/mnras/stz2822 SN - 0035-8711 SN - 1365-2966 VL - 490 IS - 3 SP - 4368 EP - 4381 PB - Oxford Univ. Press CY - Oxford ER - TY - JOUR A1 - Charpinet, Stéphane A1 - Brassard, P. A1 - Fontaine, G. A1 - Van Grootel, Valerie A1 - Zong, Weika A1 - Giammichele, N. A1 - Heber, Ulrich A1 - Bognár, Zsófia A1 - Geier, Stephan A1 - Green, Elizabeth M. A1 - Hermes, J. J. A1 - Kilkenny, D. A1 - Ostensen, R. H. A1 - Pelisoli, Ingrid Domingos A1 - Silvotti, R. A1 - Telting, J. H. A1 - Vuckovic, Maja A1 - Worters, H. L. A1 - Baran, Andrzej S. A1 - Bell, Keaton J. A1 - Bradley, Paul A. A1 - Debes, J. H. A1 - Kawaler, S. D. A1 - Kolaczek-Szymanski, P. A1 - Murphy, S. J. A1 - Pigulski, A. A1 - Sodor, A. A1 - Uzundag, Murat A1 - Handberg, R. A1 - Kjeldsen, H. A1 - Ricker, G. R. A1 - Vanderspek, R. K. T1 - TESS first look at evolved compact pulsators Discovery and asteroseismic probing of the g-mode hot B subdwarf pulsator EC 21494-7018 JF - Astronomy and astrophysics : an international weekly journal N2 - Context. The TESS satellite was launched in 2018 to perform high-precision photometry from space over almost the whole sky in a search for exoplanets orbiting bright stars. This instrument has opened new opportunities to study variable hot subdwarfs, white dwarfs, and related compact objects. Targets of interest include white dwarf and hot subdwarf pulsators, both carrying high potential for asteroseismology. Aims. We present the discovery and detailed asteroseismic analysis of a new g-mode hot B subdwarf (sdB) pulsator, EC 21494-7018 (TIC 278659026), monitored in TESS first sector using 120-s cadence. Methods. The TESS light curve was analyzed with standard prewhitening techniques, followed by forward modeling using our latest generation of sdB models developed for asteroseismic investigations. By simultaneously best-matching all the observed frequencies with those computed from models, we identified the pulsation modes detected and, more importantly, we determined the global parameters and structural configuration of the star. Results. The light curve analysis reveals that EC 21494-7018 is a sdB pulsator counting up to 20 frequencies associated with independent g-modes. The seismic analysis singles out an optimal model solution in full agreement with independent measurements provided by spectroscopy (atmospheric parameters derived from model atmospheres) and astrometry (distance evaluated from Gaia DR2 trigonometric parallax). Several key parameters of the star are derived. Its mass (0.391 +/- 0.009x2006;M-circle dot) is significantly lower than the typical mass of sdB stars and suggests that its progenitor has not undergone the He-core flash; therefore this progenitor could originate from a massive (greater than or similar to 2;M-circle dot) red giant, which is an alternative channel for the formation of sdBs. Other derived parameters include the H-rich envelope mass (0.0037 +/- 0.0010;M-circle dot), radius (0.1694 +/- 0.0081;R-circle dot), and luminosity (8.2 +/- 1.1;L-circle dot). The optimal model fit has a double-layered He+H composition profile, which we interpret as an incomplete but ongoing process of gravitational settling of helium at the bottom of a thick H-rich envelope. Moreover, the derived properties of the core indicate that EC 21494-7018 has burnt similar to 43% (in mass) of its central helium and possesses a relatively large mixed core (M-core;=;0.198 +/- 0.010;M-circle dot), in line with trends already uncovered from other g-mode sdB pulsators analyzed with asteroseismology. Finally, we obtain for the first time an estimate of the amount of oxygen (in mass; X(O)(core) = 0.16(-0.05)(+0.13)X(O)core=0.16-0.05+0.13$ X(mathrm{O})_{mathrm{core}}=0.16_{-0.05}<^>{+0.13} $) produced at this stage of evolution by an helium-burning core. This result, along with the core-size estimate, is an interesting constraint that may help to narrow down the still uncertain C-12(alpha,;gamma)O-16 nuclear reaction rate. KW - asteroseismology KW - stars KW - interiors KW - oscillations KW - horizontal-branch KW - individual KW - TIC 278659026 KW - subdwarfs Y1 - 2019 U6 - https://doi.org/10.1051/0004-6361/201935395 SN - 0004-6361 SN - 1432-0746 VL - 632 PB - EDP Sciences CY - Les Ulis ER - TY - JOUR A1 - Codutti, Agnese A1 - Bente, Klaas A1 - Faivre, Damien A1 - Klumpp, Stefan T1 - Chemotaxis in external fields: Simulations for active magnetic biological matter JF - PLoS Computational Biology : a new community journal N2 - The movement of microswimmers is often described by active Brownian particle models. Here we introduce a variant of these models with several internal states of the swimmer to describe stochastic strategies for directional swimming such as run and tumble or run and reverse that are used by microorganisms for chemotaxis. The model includes a mechanism to generate a directional bias for chemotaxis and interactions with external fields (e.g., gravity, magnetic field, fluid flow) that impose forces or torques on the swimmer. We show how this modified model can be applied to various scenarios: First, the run and tumble motion of E. coli is used to establish a paradigm for chemotaxis and investigate how it is affected by external forces. Then, we study magneto-aerotaxis in magnetotactic bacteria, which is biased not only by an oxygen gradient towards a preferred concentration, but also by magnetic fields, which exert a torque on an intracellular chain of magnets. We study the competition of magnetic alignment with active reorientation and show that the magnetic orientation can improve chemotaxis and thereby provide an advantage to the bacteria, even at rather large inclination angles of the magnetic field relative to the oxygen gradient, a case reminiscent of what is expected for the bacteria at or close to the equator. The highest gain in chemotactic velocity is obtained for run and tumble with a magnetic field parallel to the gradient, but in general a mechanism for reverse motion is necessary to swim against the magnetic field and a run and reverse strategy is more advantageous in the presence of a magnetic torque. This finding is consistent with observations that the dominant mode of directional changes in magnetotactic bacteria is reversal rather than tumbles. Moreover, it provides guidance for the design of future magnetic biohybrid swimmers. Author summary In this paper, we propose a modified Active Brownian particle model to describe bacterial swimming behavior under the influence of external forces and torques, in particular of a magnetic torque. This type of interaction is particularly important for magnetic biohybrids (i.e. motile bacteria coupled to a synthetic magnetic component) and for magnetotactic bacteria (i.e. bacteria with a natural intracellular magnetic chain), which perform chemotaxis to swim along chemical gradients, but are also directed by an external magnetic field. The model allows us to investigate the benefits and disadvantages of such coupling between two different directionality mechanisms. In particular we show that the magnetic torque can speed chemotaxis up in some conditions, while it can hinder it in other cases. In addition to an understanding of the swimming strategies of naturally magnetotactic organisms, the results may guide the design of future biomedical devices. Y1 - 2019 U6 - https://doi.org/10.1371/journal.pcbi.1007548 SN - 1553-734X SN - 1553-7358 VL - 15 IS - 12 PB - PLoS CY - San Fransisco ER - TY - JOUR A1 - Jain, Varun A1 - Wheeler, Joshua J. A1 - Ess, Daniel H. A1 - Noack, Sebastian A1 - Vacogne, Charlotte D. A1 - Schlaad, Helmut A1 - Bahr, Stephan A1 - Dietrich, Paul A1 - Meyer, Michael A1 - Thissen, Andreas A1 - Linford, Matthew R. T1 - Poly(gamma-benzyl l-glutamate), by near-ambient pressure XPS JF - Surface science spectra : SSS : an international journal & database devoted to archiving spectra from surfaces & interfaces N2 - Near-ambient pressure x-ray photoelectron spectroscopy (NAP-XPS) is a less traditional form of XPS that allows samples to be analyzed at relatively high pressures, i. e., at greater than 2500 Pa. In this study, poly(.- benzyl L- glutamate) (PBLG) with a molar mass of 11.3 kg/mol was analyzed by NAP-XPS; here, we show the survey, C 1s, N 1s, and O 1s narrow scans of PBLG. The C 1s peak envelope was fitted in three different ways, to five, six, or seven synthetic peaks. In each fit, there was also a shake-up signal. The O 1s narrow scan was well fit with three peaks: CZO and CvO in a 1:2 ratio from the polymer, and a higher energy signal from water vapor. Hartree-Fock orbital energies of a model monomer served as a guide to an additional fit of the C 1s envelope. KW - near-ambient pressure x-ray photoelectron spectroscopy KW - NAP-XPS KW - XPS KW - polymer KW - poly(gamma-benzyl L-glutamate) KW - PBLG Y1 - 2019 U6 - https://doi.org/10.1116/1.5109121 SN - 1055-5269 SN - 1520-8575 VL - 26 IS - 2 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Petitgirard, Sylvain A1 - Spiekermann, Georg A1 - Glazyrin, Konstantin A1 - Garrevoet, Jan A1 - Murakami, Motohiko T1 - Density of amorphous GeO2 to 133 GPa with possible pyritelike structure and stiffness at high pressure JF - Physical review : B, Condensed matter and materials physics N2 - Germanium oxide is a prototype network-forming oxide with pressure-induced structural changes similar to those found in crystals and amorphous silicate oxides at high pressure. Studying density and coordination changes in amorphous GeO2 allows for insight into structural changes in silicate oxides at very high pressure, with implications for the properties of planetary magmas. Here, we report the density of germanium oxide glass up to 133 GPa using the x-ray absorption technique, with very good agreement with previous experimental data at pressure below 40 GPa and recent calculation up to 140 GPa. Our data highlight four distinct compressibility domains, corresponding to changes of the local structure of GeO2. Above 80 GPa, our density data show a compressibility and bulk modulus similar to the counterpart crystal phase, and we propose that a compact distorted sixfold coordination, similar to the structural motif of the pyritelike crystalline GeO2 polymorph, is likely to be stable in that pressure range. Our density data point to a smooth continuous evolution of the average coordination for pressure above 20 GPa with persistent sixfold coordination, without sharp density or density slope discontinuities. These observations are in very good agreement with theoretical calculations and spectroscopic measurements, and our results indicate that glasses and melts may behave similarly to their high-pressure solid counterparts with comparable densities, compressibility, and possibly average coordination. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevB.100.214104 SN - 2469-9950 SN - 2469-9969 VL - 100 IS - 21 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Krämer, Hauke Kai A1 - Marwan, Norbert T1 - Border effect corrections for diagonal line based recurrence quantification analysis measures JF - Modern physics letters : A, Particles and fields, gravitation, cosmology, nuclear physics N2 - Recurrence Quantification Analysis (RQA) defines a number of quantifiers, which base upon diagonal line structures in the recurrence plot (RP). Due to the finite size of an RP, these lines can be cut by the borders of the RP and, thus, bias the length distribution of diagonal lines and, consequently, the line based RQA measures. In this letter we investigate the impact of the mentioned border effects and of the thickening of diagonal lines in an RP (caused by tangential motion) on the estimation of the diagonal line length distribution, quantified by its entropy. Although a relation to the Lyapunov spectrum is theoretically expected, the mentioned entropy yields contradictory results in many studies. Here we summarize correction schemes for both, the border effects and the tangential motion and systematically compare them to methods from the literature. We show that these corrections lead to the expected behavior of the diagonal line length entropy, in particular meaning zero values in case of a regular motion and positive values for chaotic motion. Moreover, we test these methods under noisy conditions, in order to supply practical tools for applied statistical research. KW - Recurrence plots KW - Recurrence quantification analysis KW - Shannon entropy KW - Dynamical invariants Y1 - 2019 U6 - https://doi.org/10.1016/j.physleta.2019.125977 SN - 0375-9601 SN - 1873-2429 VL - 383 IS - 34 PB - Elsevier CY - Amsterdam ER - TY - GEN A1 - Goychuk, Igor T1 - Comment on "Anomalous Escape Governed by Thermal 1/f Noise" Reply (R. K. Singh) T2 - Physical review letters Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevLett.123.238902 SN - 0031-9007 SN - 1079-7114 VL - 123 IS - 23 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Willig, Lisa A1 - Reppert, Alexander von A1 - Deb, Marwan A1 - Ganss, F. A1 - Hellwig, O. A1 - Bargheer, Matias T1 - Finite-size effects in ultrafast remagnetization dynamics of FePt JF - Physical review : B, Condensed matter and materials physics N2 - We investigate the ultrafast magnetization dynamics of FePt in the L1(0) phase after an optical heating pulse, as used in heat-assisted magnetic recording. We compare continuous and nano-granular thin films and emphasize the impact of the finite size on the remagnetization dynamics. The remagnetization speeds up significantly with increasing external magnetic field only for the continuous film, where domain-wall motion governs the dynamics. The ultrafast remagnetization dynamics in the continuous film are only dominated by heat transport in the regime of high magnetic fields, whereas the timescale required for cooling is prevalent in the granular film for all magnetic field strengths. These findings highlight the necessary conditions for studying the intrinsic heat transport properties in magnetic materials. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevB.100.224408 SN - 2469-9950 SN - 2469-9969 VL - 100 IS - 22 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Deb, Marwan A1 - Popova, Elena A1 - Keller, Niels T1 - Different magneto-optical response of magnetic sublattices as a function of temperature in ferrimagnetic bismuth iron garnet films JF - Physical review : B, Condensed matter and materials physics N2 - In this paper we investigate the magneto-optical (MO) and magnetic properties of bismuth iron garnet Bi3Fe5O12 thin films over a wide range of photon energies (1.6-3.5 eV) and temperatures (5-740 K). Depending on the photon energy range, the Faraday rotation (Theta(F)) and ellipticity (epsilon(F)) vary nonmonotonously with temperature. This behavior cannot be explained by a magnetization variation that can only decrease with increasing temperature. Theta(F) and epsilon(F) spectra have therefore been analyzed using a model based on two optical transitions of a diamagnetic nature, representing the tetrahedral and octahedral iron sites. Thus, the contribution of each magnetic sublattice has been extracted from the global macroscopic MO response and investigated as a function of temperature. The magnetic properties of octahedral and tetrahedral sublattices depend differently on temperature, suggesting a different anisotropy due to oxygen coordination. We have demonstrated that this relatively simple macroscopic measurement with a subsequent analysis can grant access to the information on the properties at a microscopic level. These results can advance the fundamental understanding of MO properties in multisublattice magnetic materials. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevB.100.224410 SN - 2469-9950 SN - 2469-9969 VL - 100 IS - 22 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Rosenblum, Michael A1 - Pikovskij, Arkadij T1 - Nonlinear phase coupling functions: a numerical study JF - Philosophical Transactions of the Royal Society of London, Series A : Mathematical, Physical and Engineering Sciences N2 - Phase reduction is a general tool widely used to describe forced and interacting self-sustained oscillators. Here, we explore the phase coupling functions beyond the usual first-order approximation in the strength of the force. Taking the periodically forced Stuart-Landau oscillator as the paradigmatic model, we determine and numerically analyse the coupling functions up to the fourth order in the force strength. We show that the found nonlinear phase coupling functions can be used for predicting synchronization regions of the forced oscillator. KW - phase approximation KW - coupling function KW - phase response curve Y1 - 2019 U6 - https://doi.org/10.1098/rsta.2019.0093 SN - 1364-503X SN - 1471-2962 VL - 377 IS - 2160 PB - Royal Society CY - London ER - TY - JOUR A1 - Feldmann, David A1 - Arya, Pooja A1 - Lomadze, Nino A1 - Kopyshev, Alexey A1 - Santer, Svetlana T1 - Light-driven motion of self-propelled porous Janus particles JF - Applied physics letters N2 - We introduce a versatile mechanism of light-driven self-propelled motion applied to porous Janus-type particles. The mechanism is based on the generation of local light-driven diffusio-osmotic (l-LDDO) flow around each single porous particle subjected to suitable irradiation conditions. The photosensitivity is introduced by a cationic azobenzene containing surfactant, which undergoes a photoisomerization reaction from a more hydrophobic trans-state to a rather hydrophilic cis-state under illumination with light. The negatively charged porous silica particles are dispersed in a corresponding aqueous solution and absorb molecules in their trans-state but expel them in their cis-state. During illumination with blue light triggering both trans-cis and cis-trans isomerization at the same time, the colloids start to move due to the generation of a steady-state diffusive flow of cis-isomers out of and trans-isomers into the particle. This is because a hemi-spherical metal cap partially sealing the colloid breaks the symmetry of the otherwise radially directed local flow around the particle, leading to self-propelled motion. Janus particles exhibit superdiffusive motion with a velocity of similar to 0.5 mu m/s and a persistence length of ca. 50 mu m, confined to microchannels the direction can be maintained up to 300 mu m before rotational diffusion reverts it. Particles forming dimers of different shapes can be made to travel along circular trajectories. The unique feature of this mechanism is that the strength of self-propulsion can be tuned by convenient external optical stimuli (intensity and irradiation wavelength) such that a broad variety of experimental situations can be realized in a spatiotemporal way and in situ. Y1 - 2019 U6 - https://doi.org/10.1063/1.5129238 SN - 0003-6951 SN - 1077-3118 VL - 115 IS - 26 PB - American Institute of Physics CY - Melville ER - TY - THES A1 - Thiede, Tobias T1 - A multiscale analysis of additively manufactured lattice structures T1 - Multiskalige Analyse von Additiv Gefertigten Gitterstrukturen N2 - Additive Manufacturing (AM) in terms of laser powder-bed fusion (L-PBF) offers new prospects regarding the design of parts and enables therefore the production of lattice structures. These lattice structures shall be implemented in various industrial applications (e.g. gas turbines) for reasons of material savings or cooling channels. However, internal defects, residual stress, and structural deviations from the nominal geometry are unavoidable. In this work, the structural integrity of lattice structures manufactured by means of L-PBF was non-destructively investigated on a multiscale approach. A workflow for quantitative 3D powder analysis in terms of particle size, particle shape, particle porosity, inter-particle distance and packing density was established. Synchrotron computed tomography (CT) was used to correlate the packing density with the particle size and particle shape. It was also observed that at least about 50% of the powder porosity was released during production of the struts. Struts are the component of lattice structures and were investigated by means of laboratory CT. The focus was on the influence of the build angle on part porosity and surface quality. The surface topography analysis was advanced by the quantitative characterisation of re-entrant surface features. This characterisation was compared with conventional surface parameters showing their complementary information, but also the need for AM specific surface parameters. The mechanical behaviour of the lattice structure was investigated with in-situ CT under compression and successive digital volume correlation (DVC). The deformation was found to be knot-dominated, and therefore the lattice folds unit cell layer wise. The residual stress was determined experimentally for the first time in such lattice structures. Neutron diffraction was used for the non-destructive 3D stress investigation. The principal stress directions and values were determined in dependence of the number of measured directions. While a significant uni-axial stress state was found in the strut, a more hydrostatic stress state was found in the knot. In both cases, strut and knot, seven directions were at least needed to find reliable principal stress directions. N2 - Das Laserstrahlschmelzen (L-PBF) als Prozess im Bereich der Additiven Fertigung (AM) ermöglicht ein neuartiges Bauteildesign und somit auch die Produktion von komplexen Gitterstrukturen, welche Materialeinsparungen und effizientere Kühlsysteme erlauben und daher für verschiedene industrielle Anwendungen (z.B. Gasturbinen) geeignet sind. Interne Defekte, Eigenspannungen und geometrische Abweichungen von der Soll-Geometrie sind jedoch unvermeidbar. Im Rahmen dieser Arbeit wird die strukturelle Integrität von L-PBF gefertigten Gitterstrukturen zerstörungsfrei auf verschiedenen Größenskalen untersucht. Eine Auswerteroutine für dreidimensionale quantitative Pulvercharakterisierung hinsichtlich der Partikelgröße, der -form, der -porosität, des Interpartikelabstands und der Packungsdichte wurde entwickelt. Synchrotron Computertomographie (CT) wurde für die Korrelation der Packungsdichte mit der Partikelgröße und -form genutzt. Darüber hinaus konnte festgestellt werden, dass mindestens 50% der Porosität aus den Pulverpartikel während der Herstellung der Streben mittels L-PBF gelöst wurde. Streben sind die Grundbausteine der Gitterstrukturen und wurden mit industrieller CT untersucht. Dabei lag der Fokus auf dem Einfluss des Bauwinkels auf die Strebenporosität und -oberflächenqualität. Die Analyse der Oberflächentopographie wurde hinsichtlich einer quantitativen Analyse von sogenannten re-entrant features erweitert. Der Vergleich dieser Auswertung mit konventionellen Oberflächenparametern offenbarte sowohl deren Komplementarität also auch den Bedarf an neuen AM-spezifischen Oberflächenparametern. In-situ CT Versuche mit anschließender digitaler Volumenkorrelation (DVC) erlaubte die Gitterstruktur bezüglich des mechanischen Verhaltens unter Druckspannung zu bewerten. Aufgrund einer schichtweisen Faltung der Einheitszellen konnte dabei das Versagensverhalten als knoten-dominiert identifiziert werden. Mittels Neutronenbeugung konnten Eigenspannungen in solchen Gitterstrukturen erstmalig experimentell bestimmt werden. Dabei wurden sowohl die Hauptspannungsrichtungen als auch die -beträge in Abhängigkeit von der Anzahl der gemessenen Spannungsrichtungen bestimmt. Während in der Strebe ein signifikanter uni-axialer Spannungszustand nachgewiesen wurde, zeigte der Knotenpunkt einen hydrostatischeren Spannungszustand. Sowohl im Falle der Strebe als auch des Knotenpunkts waren mindestens sieben gemessene Spannungsrichtungen nötig, um die Hauptspannungsrichtungen verlässlich zu ermitteln. KW - additive manufacturing KW - laser powder bed fusion KW - computed tomography KW - neutron diffraction KW - in-situ testing KW - residual stress KW - roughness KW - powder particle analysis KW - additive Fertigung KW - Laserstrahlschmelzen KW - Computertomographie KW - Neutronendiffraktion KW - In-situ Experimente KW - Eigenspannung KW - Rauheit KW - Pulverpartikelanalyse Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-470418 ER - TY - BOOK A1 - Feldmeier, Achim T1 - Theoretical Fluid Dynamics T3 - Theoretical and Mathematical Physics Y1 - 2019 SN - 978-3-030-31021-9 (online) SN - 978-3-030-31023-3 (print) U6 - https://doi.org/10.1007/978-3-030-31022-6 PB - Springer CY - Cham ER - TY - JOUR A1 - Hofmann, Alexander J. L. A1 - Züfle, Simon A1 - Shimizu, Kohei A1 - Schmid, Markus A1 - Wessels, Vivien A1 - Jäger, Lars A1 - Altazin, Stephane A1 - Ikegami, Keitaro A1 - Khan, Motiur Rahman A1 - Neher, Dieter A1 - Ishii, Hisao A1 - Ruhstaller, Beat A1 - Brütting, Wolfgang T1 - Dipolar Doping of Organic Semiconductors to Enhance Carrier Injection JF - Physical review applied N2 - If not oriented perfectly isotropically, the strong dipole moment of polar organic semiconductor materials such as tris-(8-hydroxyquinolate)aluminum (Alq3) will lead to the buildup of a giant surface potential (GSP) and thus to a macroscopic dielectric polarization of the organic film. Despite this having been a known fact for years, the implications of such high potentials within an organic layer stack have only been studied recently. In this work, the influence of the GSP on hole injection into organic layers is investigated. Therefore, we apply a concept called dipolar doping to devices consisting of the prototypical organic materials N,N′-Di(1-naphthyl)-N,N′-diphenyl-(1,1′-biphenyl)-4,4′-diamine (NPB) as nonpolar host and Alq3 as dipolar dopant with different mixing ratios to tune the GSP. The mixtures are investigated in single-layer monopolar devices as well as bilayer metal/insulator/semiconductor structures. Characterization is done electrically using current-voltage (I-V) characteristics, impedance spectroscopy, and charge extraction by linearly increasing voltage and time of flight, as well as with ultraviolet photoelectron spectroscopy. We find a maximum in device performance for moderate to low doping concentrations of the polar species in the host. The observed behavior can be described on the basis of the Schottky effect for image-force barrier lowering, if the changes in the interface dipole, the carrier mobility, and the GSP induced by dipolar doping are taken into account. KW - Carrier dynamics KW - Electric polarization KW - Optoelectronics KW - Organic electronics KW - Doped semiconductors KW - Interfaces KW - Organic LEDs KW - Organic semiconductors Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevApplied.12.064052 SN - 2331-7019 VL - 12 IS - 6 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Pisoni, Stefano A1 - Stolterfoht, Martin A1 - Lockinger, Johannes A1 - Moser, Thierry A1 - Jiang, Yan A1 - Caprioglio, Pietro A1 - Neher, Dieter A1 - Buecheler, Stephan A1 - Tiwari, Ayodhya N. T1 - On the origin of open-circuit voltage losses in flexible n-i-p perovskite solar cells JF - Science and technology of advanced materials : STAM N2 - The possibility to manufacture perovskite solar cells (PSCs) at low temperatures paves the way to flexible and lightweight photovoltaic (PV) devices manufactured via high-throughput roll-to-roll processes. In order to achieve higher power conversion efficiencies, it is necessary to approach the radiative limit via suppression of non-radiative recombination losses. Herein, we performed a systematic voltage loss analysis for a typical low-temperature processed, flexible PSC in n-i-p configuration using vacuum deposited C-60 as electron transport layer (ETL) and two-step hybrid vacuum-solution deposition for CH3NH3PbI3 perovskite absorber. We identified the ETL/absorber interface as a bottleneck in relation to non-radiative recombination losses, the quasi-Fermi level splitting (QFLS) decreases from similar to 1.23 eV for the bare absorber, just similar to 90 meV below the radiative limit, to similar to 1.10 eV when C-60 is used as ETL. To effectively mitigate these voltage losses, we investigated different interfacial modifications via vacuum deposited interlayers (BCP, B4PyMPM, 3TPYMB, and LiF). An improvement in QFLS of similar to 30-40 meV is observed after interlayer deposition and confirmed by comparable improvements in the open-circuit voltage after implementation of these interfacial modifications in flexible PSCs. Further investigations on absorber/hole transport layer (HTL) interface point out the detrimental role of dopants in Spiro-OMeTAD film (widely employed HTL in the community) as recombination centers upon oxidation and light exposure. [GRAPHICS] . KW - Perovskite solar cell KW - flexible KW - interface engineering KW - non-radiative recombination KW - quasi-Fermi level splitting Y1 - 2019 U6 - https://doi.org/10.1080/14686996.2019.1633952 SN - 1468-6996 SN - 1878-5514 VL - 20 SP - 786 EP - 795 PB - Taylor & Francis CY - Abingdon ER - TY - THES A1 - Nguyen, Quyet Doan T1 - Electro-acoustical probing of space-charge and dipole-polarization profiles in polymer dielectrics for electret and electrical-insulation applications T1 - Elektroakustische Abtastung von elektrischen Ladungs- und Polarisationsprofilen in Polymerfolien für Elektret- und Isolations-Anwendungen N2 - Electrets are dielectrics with quasi-permanent electric charge and/or dipoles, sometimes can be regarded as an electric analogy to a magnet. Since the discovery of the excellent charge retention capacity of poly(tetrafluoro ethylene) and the invention of the electret microphone, electrets have grown out of a scientific curiosity to an important application both in science and technology. The history of electret research goes hand in hand with the quest for new materials with better capacity at charge and/or dipole retention. To be useful, electrets normally have to be charged/poled to render them electro-active. This process involves electric-charge deposition and/or electric dipole orientation within the dielectrics ` surfaces and bulk. Knowledge of the spatial distribution of electric charge and/or dipole polarization after their deposition and subsequent decay is crucial in the task to improve their stability in the dielectrics. Likewise, for dielectrics used in electrical insulation applications, there are also needs for accumulated space-charge and polarization spatial profiling. Traditionally, space-charge accumulation and large dipole polarization within insulating dielectrics is considered undesirable and harmful to the insulating dielectrics as they might cause dielectric loss and could lead to internal electric field distortion and local field enhancement. High local electric field could trigger several aging processes and reduce the insulating dielectrics' lifetime. However, with the advent of high-voltage DC transmission and high-voltage capacitor for energy storage, these are no longer the case. There are some overlapped between the two fields of electrets and electric insulation. While quasi-permanently trapped electric-charge and/or large remanent dipole polarization are the requisites for electret operation, stably trapped electric charge in electric insulation helps reduce electric charge transport and overall reduced electric conductivity. Controlled charge trapping can help in preventing further charge injection and accumulation as well as serving as field grading purpose in insulating dielectrics whereas large dipole polarization can be utilized in energy storage applications. In this thesis, the Piezoelectrically-generated Pressure Steps (PPSs) were employed as a nondestructive method to probe the electric-charge and dipole polarization distribution in a range of thin film (several hundred micron) polymer-based materials, namely polypropylene (PP), low-density polyethylene/magnesium oxide (LDPE/MgO) nanocomposites and poly(vinylidene fluoride-co- trifluoro ethylene) (P(VDF-TrFE)) copolymer. PP film surface-treated with phosphoric acid to introduce surfacial isolated nanostructures serves as example of 2-dimensional nano-composites whereas LDPE/MgO serves as the case of 3-dimensional nano-composites with MgO nano-particles dispersed in LDPE polymer matrix. It is evidenced that the nanoparticles on the surface of acid-treated PP and in the bulk of LDPE/MgO nanocomposites improve charge trapping capacity of the respective material and prevent further charge injection and transport and that the enhanced charge trapping capacity makes PP and LDPE/MgO nanocomposites potential materials for both electret and electrical insulation applications. As for PVDF and VDF-based copolymers, the remanent spatial polarization distribution depends critically on poling method as well as specific parameters used in the respective poling method. In this work, homogeneous polarization poling of P(VDF-TrFE) copolymers with different VDF-contents have been attempted with hysteresis cyclical poling. The behaviour of remanent polarization growth and spatial polarization distribution are reported and discussed. The Piezoelectrically-generated Pressure Steps (PPSs) method has proven as a powerful method for the charge storage and transport characterization of a wide range of polymer material from nonpolar, to polar, to polymer nanocomposites category. N2 - Elektrete sind Dielektrika mit quasi-permanenter elektrischer Ladung und/oder quasi-permanent ausgerichteten elektrischen Dipolen - das elektrische Analogon zu einem Magneten. Seit der Entdeckung der besonders hohen Stabilitaet negativer Raumladungen in Polytetrafluorethylen (PTFE, Handelsname Teflon) und der Erfindung des Elektretmikrofons ist aus der spannenden wissenschaftlichen Fragestellung nach den Ursachen der hervorragenden Ladungsspeicherung in Elektreten auch eine wichtige technische Anwendung geworden. In der Geschichte der Elektretforschung und der Elektretanwendungen geht es neben der Ursachenklaerung auch immer um die Suche nach neuen Materialien mit besserer Ladungsspeicherung und/oder Dipolpolarisation. Elektretmaterialien muessen in der Regel elektrisch aufgeladen oder gepolt werden, um die gewuenschten elektroaktiven Eigenschaften zu erhalten. Dabei werden entweder elektrische Ladungen auf der Oberflaeche oder im Volumen des Elektretmaterials deponiert und/oder elektrische Dipole im Material ausgerichtet. Genaue Informationen ueber die raeumliche Verteilung der elektrischen Ladungen und/oder der Dipolpolarisation sowie deren Entwicklung im Laufe der Zeit sind entscheidend fuer eine gezielte Verbesserung der Elektretstabilitaet. Dielektrika, die zur elektrischen Isolierung von Hochspannungsanlagen eingesetzt werden, koennen ebenfalls elektrische Raumladungen und/oder Dipolpolarisationen enthalten, deren Verteilungen entscheidend fuer die Beherrschung der damit einhergehenden Eigenschaftsaenderungen sind. Traditionell gelten Raumladungen und Dipolpolarisationen in elektrischen Isolierungen als unerwuenscht und schaedlich, da sie zu erheblichen Verlusten und zu Verzerrungen der inneren elektrischen Felder fuehren koennen. Hohe lokale Felder koennen Alterungsprozesse ausloesen und die Lebensdauer der isolierenden Dielektrika erheblich verkuerzen. Mit dem Aufkommen der Hochspannungs-Gleichstromuebertragung und des Hochspannungskondensators zur Energiespeicherung in den letzten Jahren hat sich die Situation jedoch grundlegend geaendert, da Raumladungen prinzipiell nicht mehr vermeidbar sind und bei entsprechender Gestaltung der Isolierung moeglicherweise sogar von Vorteil sein koennen. Hier ergeben sich nun Ueberschneidungen und Synergien zwischen Elektreten und elektrischen Isoliermaterialien, zumal in beiden Faellen hohe elektrische Gleichfelder auftreten. Waehrend quasi-permanent gespeicherte elektrische Ladungen und/oder stark quasi- permanente oder remanente Dipolpolarisationen das wesentliche Merkmal von Elektreten sind, koennen stabil gespeicherte elektrische Ladungen in elektrischen Isolierungen dazu beitragen, den schaedlichen Ladungstransport und damit die effektive elektrische Leitfaehigkeit der Dielektrika zu reduzieren. Ein kontrolliertes Einbringen von Raumladungen kann die Injektion und die Anhaeufung weiterer Ladungen verhindern, waehrend stark Dipolpolarisationen die Kapazitaet von elektrischen Energiespeichern wesentlich erhoehen koennen. In der vorliegenden Arbeit wurden piezoelektrisch erzeugte Druckstufen (Piezoelectrically generated Pressure Steps oder PPSs) eingesetzt, um die Verteilung elektrischer Ladungen und/oder ausgerichteter elektrischer Dipole in relativ duennen polymeren Dielektrika (Mikrometerbereich) zu untersuchen. Wesentliche Probenmaterialien waren Polypropylen (PP), Komposite aus Polyethylen mit Magnesiumoxid-Nanopartikeln in geringen Mengen (LDPE/MgO) sowie Poly(vinyliden fluorid-trifluorethylen)-Copolymere (P(VDF-TrFE)). PP-Folien, die mit Phosphorsaeure oberflaechenbehandelt wurden, um voneinander isolierte Nanostrukturen an der Oberflaeche zu erzeugen, sind ein Beispiel fuer ein zweidimensionales (2-D) Nanokomposit, waehrend LDPE/MgO ein dreidimensionales (3-D) Nanokomposit darstellt. Es konnte nachgewiesen werden, dass die Nanopartikel auf der Oberflaeche von saeurebehandeltem PP und im Volumen von LDPE/MgO-Nanokompositen die Ladungsspeicherfaehigkeit des jeweiligen Materials entscheidend verbessern. Damit werden weitere Ladungsinjektionen und der Ladungstransport verhindert, was die 2-D PP- und die 3-D LDPE/MgO-Nanokomposite zu geeigneten Kandidaten sowohl fuer Elektret- als auch fuer Isolationsanwendungen macht. Bei Polyvinylidenfluorid (PVDF) und Copolymeren auf der Basis von Vinylidenfluorid (VDF) haengt die remanente raeumliche Polarisationsverteilung entscheidend von der jeweiligen Polungsmethode sowie von den Parametern des jeweiligen Polungsvorgangs ab. Hier wurde versucht, eine homogene Polung von P(VDF-TrFE)-Copolymeren mit unterschiedlichen VDF-Gehalten mit dem Verfahren der zyklischen Polung (sogenannte Hysterese-Polung) zu erzeugen. Das Entstehen der remanenten Polarisation und deren raeumliche Verteilung konnten erfasst und interpretiert werden, um Hinweise für eine optimale Polung zu erhalten. An den genannten Beispielen konnte gezeigt werden, dass die Methode der piezoelektrisch erzeugten Druckstufen (PPS) ein leistungsfaehiges Verfahren zur Charakterisierung der Ladungsspeicherung und des Ladungstransports in Dielektrika ist und dass damit ein breites Spektrum von unpolaren Polymeren ueber polare Polymerdielektrika bis hin zu polaren Nanokompositen sinnvoll untersucht werden kann. Es wurden wesentliche Erkenntnisse zur Ladungsspeicherung und zur remanten Polarisation in den untersuchten Polymeren gewonnen. KW - electro-acoustic electric-charge and polarization profiling KW - space charge KW - polypropylene KW - polyethylene nanocomposites KW - magnesium oxide KW - polymer electrets KW - ferroelectrets KW - electrical insulation KW - piezoelectricity KW - ferroelectricity KW - poly(vinylidene fluoride) KW - hysteresis KW - elektroakustische Abtastung elektrischer Ladungen und Dipolpolarisationen KW - elektrische Raumladung KW - Polypropylen KW - Polyethylen-Nanokomposite KW - Magnesiumoxid KW - Polymerelektrete KW - Ferroelektrete KW - elektrische Isolierung KW - Piezoelektrizität KW - Ferroelektrizität KW - Poly(vinylidenfluorid) KW - Hysterese Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-445629 ER - TY - JOUR A1 - Grebenkov, Denis S. A1 - Metzler, Ralf A1 - Oshanin, Gleb T1 - Full distribution of first exit times in the narrow escape problem JF - New Journal of Physics N2 - In the scenario of the narrow escape problem (NEP) a particle diffuses in a finite container and eventually leaves it through a small 'escape window' in the otherwise impermeable boundary, once it arrives to this window and crosses an entropic barrier at the entrance to it. This generic problem is mathematically identical to that of a diffusion-mediated reaction with a partially-reactive site on the container's boundary. Considerable knowledge is available on the dependence of the mean first-reaction time (FRT) on the pertinent parameters. We here go a distinct step further and derive the full FRT distribution for the NEP. We demonstrate that typical FRTs may be orders of magnitude shorter than the mean one, thus resulting in a strong defocusing of characteristic temporal scales. We unveil the geometry-control of the typical times, emphasising the role of the initial distance to the target as a decisive parameter. A crucial finding is the further FRT defocusing due to the barrier, necessitating repeated escape or reaction attempts interspersed with bulk excursions. These results add new perspectives and offer a broad comprehension of various features of the by-now classical NEP that are relevant for numerous biological and technological systems. KW - narrow escape problem KW - first-passage time distribution KW - mean versus most probable reaction times KW - mixed boundary conditions Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab5de4 SN - 1367-2630 VL - 21 PB - Dt. Physikalische Ges. CY - Bad Honnef ER - TY - GEN A1 - Grebenkov, Denis S. A1 - Metzler, Ralf A1 - Oshanin, Gleb T1 - Full distribution of first exit times in the narrow escape problem T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - In the scenario of the narrow escape problem (NEP) a particle diffuses in a finite container and eventually leaves it through a small 'escape window' in the otherwise impermeable boundary, once it arrives to this window and crosses an entropic barrier at the entrance to it. This generic problem is mathematically identical to that of a diffusion-mediated reaction with a partially-reactive site on the container's boundary. Considerable knowledge is available on the dependence of the mean first-reaction time (FRT) on the pertinent parameters. We here go a distinct step further and derive the full FRT distribution for the NEP. We demonstrate that typical FRTs may be orders of magnitude shorter than the mean one, thus resulting in a strong defocusing of characteristic temporal scales. We unveil the geometry-control of the typical times, emphasising the role of the initial distance to the target as a decisive parameter. A crucial finding is the further FRT defocusing due to the barrier, necessitating repeated escape or reaction attempts interspersed with bulk excursions. These results add new perspectives and offer a broad comprehension of various features of the by-now classical NEP that are relevant for numerous biological and technological systems. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 810 KW - narrow escape problem KW - first-passage time distribution KW - mean versus most probable reaction times KW - mixed boundary conditions Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-442883 SN - 1866-8372 IS - 810 ER - TY - THES A1 - Willig, Lisa T1 - Ultrafast magneto-optical studies of remagnetisation dynamics in transition metals T1 - Ultraschnelle Magneto-Optische Studien der Remagnetisierungsdynamik von Übergangsmetallen N2 - Ultrafast magnetisation dynamics have been investigated intensely for two decades. The recovery process after demagnetisation, however, was rarely studied experimentally and discussed in detail. The focus of this work lies on the investigation of the magnetisation on long timescales after laser excitation. It combines two ultrafast time resolved methods to study the relaxation of the magnetic and lattice system after excitation with a high fluence ultrashort laser pulse. The magnetic system is investigated by time resolved measurements of the magneto-optical Kerr effect. The experimental setup has been implemented in the scope of this work. The lattice dynamics were obtained with ultrafast X-ray diffraction. The combination of both techniques leads to a better understanding of the mechanisms involved in magnetisation recovery from a non-equilibrium condition. Three different groups of samples are investigated in this work: Thin Nickel layers capped with nonmagnetic materials, a continuous sample of the ordered L10 phase of Iron Platinum and a sample consisting of Iron Platinum nanoparticles embedded in a carbon matrix. The study of the remagnetisation reveals a general trend for all of the samples: The remagnetisation process can be described by two time dependences. A first exponential recovery that slows down with an increasing amount of energy absorbed in the system until an approximately linear time dependence is observed. This is followed by a second exponential recovery. In case of low fluence excitation, the first recovery is faster than the second. With increasing fluence the first recovery is slowed down and can be described as a linear function. If the pump-induced temperature increase in the sample is sufficiently high, a phase transition to a paramagnetic state is observed. In the remagnetisation process, the transition into the ferromagnetic state is characterised by a distinct transition between the linear and exponential recovery. From the combination of the transient lattice temperature Tp(t) obtained from ultrafast X-ray measurements and magnetisation M(t) gained from magneto-optical measurements we construct the transient magnetisation versus temperature relations M(Tp). If the lattice temperature remains below the Curie temperature the remagnetisation curve M(Tp) is linear and stays below the M(T) curve in equilibrium in the continuous transition metal layers. When the sample is heated above phase transition, the remagnetisation converges towards the static temperature dependence. For the granular Iron Platinum sample the M(Tp) curves for different fluences coincide, i.e. the remagnetisation follows a similar path irrespective of the initial laser-induced temperature jump. N2 - Ultraschnelle Magnetisierungsdynamiken wurden in den letzten zwei Jahrzehnten intensiv untersucht. Hingegen der Wiederherstellungsprozess der Magnetisierung nach einer ultraschnellen Demagnetisierung wird selten experimentell untersucht und im Detail diskutiert. Der Fokus dieser Arbeit liegt auf der Untersuchung der Magnetisierung auf langen Zeitskalen nach der Anregung durch einen Laserpuls. Dazu werden zwei ultraschnelle zeitaufgelöste Techniken verwendet, um die Relaxierung von dem magnetischen System und dem System des Gitters nach Anregung mit einem hochenergetischen ultrakurzen Laserpuls zu untersuchen. Das magnetische System wurde untersucht mithilfe von Messungen des zeitaufgelösten magneto-optischen Kerr Effekts. Der experimentelle Aufbau wurde im Rahmen dieser Arbeit entwickelt. Die Gitterdynamik wurde mittels ultraschneller Röntgendiffraktometrie aufgenommen. Die Kombination beider Techniken liefert ein besseres Verständnis von den Prozessen involviert in Magnetisierungsrelaxation aus einem Nicht-Gleichgewichtszustand. Drei unterschiedliche Probensysteme wurden im Rahmen dieser Arbeit untersucht: Dünne Nickel Schichten umgeben von nicht-magnetischen Schichten, eine kontinuierliche Schicht aus einer Eisen Platin Legierung und eine Probe bestehend aus Eisen Platin Nanopartikeln eingebettet in einer Kohlenstoffmatrix. Die Studie der Remagnetisierung zeigt einen generellen Trend für alle diese Systeme auf: Der Remagnetisierungsprozess kann mit zwei Zeitabhängikeiten beschrieben werden. Eine erste exponentielle Zeitabhängigkeit, die mit zunehmender Menge an absorbierter Energie verlangsamt wird bis ein lineares Verhalten beobachtet wird. Darauf folgend gibt es eine zweite exponentielle funktionale Abhängigkeit in der Zeit. Im Falle einer geringen Energieabsorption ist die erste Remagnetisierung schneller als die zweite. Mit steigender Fluenz wird die Remagnetisierung in der ersten Zeitabhängigkeit verlangsamt und kann als lineare Funktion beschrieben werden. Wenn der durch den Pump Puls induzierte Temperatursprung in der Probe ausreichend groß ist, wird ein Phasenübergang in die paramagnetische Phase beobachtet. In dem Remagnetisierungsprozess wird dieser Übergang durch einen deutlich sichtbaren Wechsel zwischen linearem und exponentiellen Verhalten sichtbar. Mithilfe der Kombination aus der von Rötngendaten gewonnener Gittertemperatur Tp(t) und der Magnetisierung M(t) erhalten wir die zeitliche Abhängigkeit der Magnetisierung von der Gittertemperatur M(Tp). Falls die Gittertemperatur unter der Curietemperatur bleibt, ist die Remagnetisierungskurve M(Tp) linear und bleibt unterhalb der statischen Gleichgewichtskurve M(T) für die kontinuierlichen Übergangsmetalle. Wenn die Probe über den Phasenübergang geheizt wird, nähert sich die Remagnetisierung der statischen Kurve an. Die transiente Remagnetisierungskurven M(Tp) der granularen Eisen Platin Probe folgen immer einem der statischen Magnetisierungskurve ähnlichen Verlauf, unabhängig von dem laser-induzierten Temperatursprung. KW - ultrafast dynamics KW - remagnetization KW - magnetization dynamics KW - transition metals KW - condensed matter KW - ultraschnelle Dynamik KW - magneto-optics KW - Magneto-Optik KW - Remagnetisierung KW - Magnetisierungsdynamik KW - Übergangsmetalle KW - kondensierte Materie Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-441942 ER - TY - THES A1 - Nagel, Oliver T1 - Amoeboid cells as a transport system for micro-objects T1 - Amöboide Zellen als Transportsystem für Mikroobjekte N2 - Due to advances in science and technology towards smaller and more powerful processing units, the fabrication of micrometer sized machines for different tasks becomes more and more possible. Such micro-robots could revolutionize medical treatment of diseases and shall support to work on other small machines. Nevertheless, scaling down robots and other devices is a challenging task and will probably remain limited in near future. Over the past decade the concept of bio-hybrid systems has proved to be a promising approach in order to advance the further development of micro-robots. Bio-hybrid systems combine biological cells with artificial components, thereby benefiting from the functionality of living biological cells. Cell-driven micro-transport is one of the most prominent applications in the emerging field of these systems. So far, micrometer sized cargo has been successfully transported by means of swimming bacterial cells. The potential of motile adherent cells as transport systems has largely remained unexplored. This thesis concentrates on the social amoeba Dictyostelium discoideum as a potential candidate for an amoeboid bio-hybrid transport system. The use of this model organism comes with several advantages. Due to the unspecific properties of Dictyostelium adhesion, a wide range of different cargo materials can be used for transport. As amoeboid cells exceed bacterial cells in size by one order of magnitude, also the size of an object carried by a single cell can also be much larger for an amoeba. Finally it is possible to guide the cell-driven transport based on the chemotactic behavior of the amoeba. Since cells undergo a developmentally induced chemotactic aggregation, cargo could be assembled in a self-organized manner into a cluster. It is also possible to impose an external chemical gradient to guide the amoeboid transport system to a desired location. To establish Dictyostelium discoideum as a possible candidate for bio-hybrid transport systems, this thesis will first investigate the movement of single cells. Secondly, the interaction of cargo and cells will be studied. Eventually, a conceptional proof will be conducted, that the cheomtactic behavior can be exploited either to transport a cargo self-organized or through an external chemical source. N2 - Durch die Fortschritte in Wissenschaft und Technik hin zu kleineren und leistungsfähigeren Prozessoren wird die Herstellung von Maschinen mit einer Größe von wenigen Mikrometern immer wahrscheinlicher. Solche Mikro-Roboter könnten sowohl die medizinische Behandlung von Krankheiten revolutionieren als auch dabei helfen andere kleine Maschinen zu bauen. Nichts desto trotz ist es eine komplizierte Aufgabe Roboter sowie andere Maschinen zu verkleinern und wird in naher Zukunft wohl nur begrenzt möglich sein. Im Verlauf des letzten Jahrzehnts hat sich das Konzept der Bio-Hybridsysteme als ein vielversprechender Ansatz entwickelt, um Mikro-Roboter weiter zu entwickeln. Bio-Hybridsysteme kombinieren biologische Zellen mit künstlichen Komponenten, um so einen Vorteil aus der Funktionalität lebender biologischer Zellen zu ziehen. Der zellgetriebene Mikro-Transport ist eine der bekanntesten Anwendungen in dem wachsenden Feld dieser Systeme. Bisher wurde mikrometergroße Fracht erfolgreich mit Hilfe von schwimmenden Bakterien transportiert. Das Potential beweglicher, adhärenter Zellen als Transportsystem blieb bisher weitgehend unerforscht. Diese Arbeit beschäftigt sich mit der sozialen Amöbe Dictyostelium discoideum als einen potentiellen Kandidaten für ein auf Amöben basiertes Bio-Hybridtransportsystem. Die Nutzung dieses Modellorganismus bringt einige Vorteile mit sich. Auf Grund der unspezifischen Adhäsion von Dictyostelium ist es möglich eine Vielzahl von verschiedenen Frachtmaterialien für den Transport zu nutzen. Da Amöben um eine Größenordnung größer sind als Bakterien, können auch die Objekte, die eine einzelne Amöbe transportieren kann um einiges größer sein, als bei einer einzelnen Bakterie. Desweiteren ist noch möglich den zellgetrieben Transport durch das chemotaktische Verhalten der Amöben zu steuern. Da die Zellen im Verlauf ihres Lebenszyklus’ eine entwicklungsinduzierte chemotaktische Aggregation durchlaufen, ist es möglich, die Fracht in einer selbstorganisierten Art und Weise in Aggregate zusammen zu führen. Es ist auch möglich einen externen chemotaktischen Stimulus zu generieren, um das auf Amöben basierende Transportsystem zu einer gewünschten Position zu lenken. Um Dictyostelium discoideum als denkbaren Kandidaten für ein Bio-Hybridtransportsystem zu etablieren, wird in dieser Arbeit zuerst die Bewegung einzelner Zellen untersucht. Als zweites wird die Interaktion von Zellen und Fracht studiert. Zum Schluss wird ein konzeptioneller Beweis geführt, dass das chemotaktische Verhalten der Zellen genutzt werden kann, um eine Fracht entweder selbstorganisiert oder mit Hilfe eines externen Stimulus zu transportieren. KW - bio-hybrid KW - dicytostelium KW - chemotaxsis KW - Bio-Hybrid KW - Dicytostelium KW - Chemotaxsis Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-442192 ER - TY - GEN A1 - Weber, Ariane A1 - Bahrs, Marco A1 - Alirezaeizanjani, Zahra A1 - Zhang, Xingyu A1 - Beta, Carsten A1 - Zaburdaev, Vasily T1 - Rectification of Bacterial Diffusion in Microfluidic Labyrinths T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - In nature as well as in the context of infection and medical applications, bacteria often have to move in highly complex environments such as soil or tissues. Previous studies have shown that bacteria strongly interact with their surroundings and are often guided by confinements. Here, we investigate theoretically how the dispersal of swimming bacteria can be augmented by microfluidic environments and validate our theoretical predictions experimentally. We consider a system of bacteria performing the prototypical run-and-tumble motion inside a labyrinth with square lattice geometry. Narrow channels between the square obstacles limit the possibility of bacteria to reorient during tumbling events to an area where channels cross. Thus, by varying the geometry of the lattice it might be possible to control the dispersal of cells. We present a theoretical model quantifying diffusive spreading of a run-and-tumble random walker in a square lattice. Numerical simulations validate our theoretical predictions for the dependence of the diffusion coefficient on the lattice geometry. We show that bacteria moving in square labyrinths exhibit enhanced dispersal as compared to unconfined cells. Importantly, confinement significantly extends the duration of the phase with strongly non-Gaussian diffusion, when the geometry of channels is imprinted in the density profiles of spreading cells. Finally, in good agreement with our theoretical findings, we observe the predicted behaviors in experiments with E. coli bacteria swimming in a square lattice labyrinth created in amicrofluidic device. Altogether, our comprehensive understanding of bacterial dispersal in a simple two-dimensional labyrinth makes the first step toward the analysis of more complex geometries relevant for real world applications. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 801 KW - diffusion KW - rectification KW - random walk KW - bacteria KW - confinement Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-441222 SN - 1866-8372 IS - 801 ER - TY - JOUR A1 - Weber, Ariane A1 - Bahrs, Marco A1 - Alirezaeizanjani, Zahra A1 - Zhang, Xingyu A1 - Beta, Carsten A1 - Zaburdaev, Vasily T1 - Rectification of Bacterial Diffusion in Microfluidic Labyrinths JF - Frontiers in Physics N2 - In nature as well as in the context of infection and medical applications, bacteria often have to move in highly complex environments such as soil or tissues. Previous studies have shown that bacteria strongly interact with their surroundings and are often guided by confinements. Here, we investigate theoretically how the dispersal of swimming bacteria can be augmented by microfluidic environments and validate our theoretical predictions experimentally. We consider a system of bacteria performing the prototypical run-and-tumble motion inside a labyrinth with square lattice geometry. Narrow channels between the square obstacles limit the possibility of bacteria to reorient during tumbling events to an area where channels cross. Thus, by varying the geometry of the lattice it might be possible to control the dispersal of cells. We present a theoretical model quantifying diffusive spreading of a run-and-tumble random walker in a square lattice. Numerical simulations validate our theoretical predictions for the dependence of the diffusion coefficient on the lattice geometry. We show that bacteria moving in square labyrinths exhibit enhanced dispersal as compared to unconfined cells. Importantly, confinement significantly extends the duration of the phase with strongly non-Gaussian diffusion, when the geometry of channels is imprinted in the density profiles of spreading cells. Finally, in good agreement with our theoretical findings, we observe the predicted behaviors in experiments with E. coli bacteria swimming in a square lattice labyrinth created in amicrofluidic device. Altogether, our comprehensive understanding of bacterial dispersal in a simple two-dimensional labyrinth makes the first step toward the analysis of more complex geometries relevant for real world applications. KW - diffusion KW - rectification KW - random walk KW - bacteria KW - confinement Y1 - 2019 U6 - https://doi.org/10.3389/fphy.2019.00148 SN - 2296-424X SN - 0429-7725 VL - 7 PB - Frontiers Media CY - Lausanne ER - TY - JOUR A1 - Palyulin, Vladimir V A1 - Blackburn, George A1 - Lomholt, Michael A A1 - Watkins, Nicholas W A1 - Metzler, Ralf A1 - Klages, Rainer A1 - Chechkin, Aleksei V. T1 - First passage and first hitting times of Lévy flights and Lévy walks JF - New Journal of Physics N2 - For both Lévy flight and Lévy walk search processes we analyse the full distribution of first-passage and first-hitting (or first-arrival) times. These are, respectively, the times when the particle moves across a point at some given distance from its initial position for the first time, or when it lands at a given point for the first time. For Lévy motions with their propensity for long relocation events and thus the possibility to jump across a given point in space without actually hitting it ('leapovers'), these two definitions lead to significantly different results. We study the first-passage and first-hitting time distributions as functions of the Lévy stable index, highlighting the different behaviour for the cases when the first absolute moment of the jump length distribution is finite or infinite. In particular we examine the limits of short and long times. Our results will find their application in the mathematical modelling of random search processes as well as computer algorithms. KW - Lévy flights KW - Lévy walks KW - first-passage time KW - first-hitting time Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab41bb SN - 1367-2630 VL - 21 PB - Dt. Physikalische Ges. CY - Bad Honnef ER - TY - GEN A1 - Palyulin, Vladimir V A1 - Blackburn, George A1 - Lomholt, Michael A A1 - Watkins, Nicholas W A1 - Metzler, Ralf A1 - Klages, Rainer A1 - Chechkin, Aleksei V. T1 - First passage and first hitting times of Lévy flights and Lévy walks T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - For both Lévy flight and Lévy walk search processes we analyse the full distribution of first-passage and first-hitting (or first-arrival) times. These are, respectively, the times when the particle moves across a point at some given distance from its initial position for the first time, or when it lands at a given point for the first time. For Lévy motions with their propensity for long relocation events and thus the possibility to jump across a given point in space without actually hitting it ('leapovers'), these two definitions lead to significantly different results. We study the first-passage and first-hitting time distributions as functions of the Lévy stable index, highlighting the different behaviour for the cases when the first absolute moment of the jump length distribution is finite or infinite. In particular we examine the limits of short and long times. Our results will find their application in the mathematical modelling of random search processes as well as computer algorithms. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 785 KW - Lévy flights KW - Lévy walks KW - first-passage time KW - first-hitting time Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-439832 SN - 1866-8372 IS - 785 ER - TY - GEN A1 - Kindler, Oliver A1 - Pulkkinen, Otto A1 - Cherstvy, Andrey G. A1 - Metzler, Ralf T1 - Burst Statistics in an Early Biofilm Quorum Sensing Mode BT - The Role of Spatial Colony-Growth Heterogeneity T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - Quorum-sensing bacteria in a growing colony of cells send out signalling molecules (so-called “autoinducers”) and themselves sense the autoinducer concentration in their vicinity. Once—due to increased local cell density inside a “cluster” of the growing colony—the concentration of autoinducers exceeds a threshold value, cells in this clusters get “induced” into a communal, multi-cell biofilm-forming mode in a cluster-wide burst event. We analyse quantitatively the influence of spatial disorder, the local heterogeneity of the spatial distribution of cells in the colony, and additional physical parameters such as the autoinducer signal range on the induction dynamics of the cell colony. Spatial inhomogeneity with higher local cell concentrations in clusters leads to earlier but more localised induction events, while homogeneous distributions lead to comparatively delayed but more concerted induction of the cell colony, and, thus, a behaviour close to the mean-field dynamics. We quantify the induction dynamics with quantifiers such as the time series of induction events and burst sizes, the grouping into induction families, and the mean autoinducer concentration levels. Consequences for different scenarios of biofilm growth are discussed, providing possible cues for biofilm control in both health care and biotechnology. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 777 Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-439099 SN - 1866-8372 IS - 777 ER - TY - JOUR A1 - Kindler, Oliver A1 - Pulkkinen, Otto A1 - Cherstvy, Andrey G. A1 - Metzler, Ralf T1 - Burst Statistics in an Early Biofilm Quorum Sensing Mode BT - The Role of Spatial Colony-Growth Heterogeneity JF - Scientific Reports N2 - Quorum-sensing bacteria in a growing colony of cells send out signalling molecules (so-called “autoinducers”) and themselves sense the autoinducer concentration in their vicinity. Once—due to increased local cell density inside a “cluster” of the growing colony—the concentration of autoinducers exceeds a threshold value, cells in this clusters get “induced” into a communal, multi-cell biofilm-forming mode in a cluster-wide burst event. We analyse quantitatively the influence of spatial disorder, the local heterogeneity of the spatial distribution of cells in the colony, and additional physical parameters such as the autoinducer signal range on the induction dynamics of the cell colony. Spatial inhomogeneity with higher local cell concentrations in clusters leads to earlier but more localised induction events, while homogeneous distributions lead to comparatively delayed but more concerted induction of the cell colony, and, thus, a behaviour close to the mean-field dynamics. We quantify the induction dynamics with quantifiers such as the time series of induction events and burst sizes, the grouping into induction families, and the mean autoinducer concentration levels. Consequences for different scenarios of biofilm growth are discussed, providing possible cues for biofilm control in both health care and biotechnology. Y1 - 2019 U6 - https://doi.org/10.1038/s41598-019-48525-2 SN - 2045-2322 VL - 9 PB - Macmillan Publishers Limited part of Springer Nature CY - London ER - TY - GEN A1 - Ślęzak, Jakub A1 - Burnecki, Krzysztof A1 - Metzler, Ralf T1 - Random coefficient autoregressive processes describe Brownian yet non-Gaussian diffusion in heterogeneous systems T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - Many studies on biological and soft matter systems report the joint presence of a linear mean-squared displacement and a non-Gaussian probability density exhibiting, for instance, exponential or stretched-Gaussian tails. This phenomenon is ascribed to the heterogeneity of the medium and is captured by random parameter models such as ‘superstatistics’ or ‘diffusing diffusivity’. Independently, scientists working in the area of time series analysis and statistics have studied a class of discrete-time processes with similar properties, namely, random coefficient autoregressive models. In this work we try to reconcile these two approaches and thus provide a bridge between physical stochastic processes and autoregressive models.Westart from the basic Langevin equation of motion with time-varying damping or diffusion coefficients and establish the link to random coefficient autoregressive processes. By exploring that link we gain access to efficient statistical methods which can help to identify data exhibiting Brownian yet non-Gaussian diffusion. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 765 KW - diffusion KW - Langevin equation KW - Brownian yet non-Gaussian diffusion KW - diffusing diffusivity KW - superstatistics KW - autoregressive models KW - time series analysis KW - codifference Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-437923 SN - 1866-8372 IS - 765 ER - TY - JOUR A1 - Ślęzak, Jakub A1 - Burnecki, Krzysztof A1 - Metzler, Ralf T1 - Random coefficient autoregressive processes describe Brownian yet non-Gaussian diffusion in heterogeneous systems JF - New Journal of Physics N2 - Many studies on biological and soft matter systems report the joint presence of a linear mean-squared displacement and a non-Gaussian probability density exhibiting, for instance, exponential or stretched-Gaussian tails. This phenomenon is ascribed to the heterogeneity of the medium and is captured by random parameter models such as ‘superstatistics’ or ‘diffusing diffusivity’. Independently, scientists working in the area of time series analysis and statistics have studied a class of discrete-time processes with similar properties, namely, random coefficient autoregressive models. In this work we try to reconcile these two approaches and thus provide a bridge between physical stochastic processes and autoregressive models.Westart from the basic Langevin equation of motion with time-varying damping or diffusion coefficients and establish the link to random coefficient autoregressive processes. By exploring that link we gain access to efficient statistical methods which can help to identify data exhibiting Brownian yet non-Gaussian diffusion. KW - diffusion KW - Langevin equation KW - Brownian yet non-Gaussian diffusion KW - diffusing diffusivity KW - superstatistics KW - autoregressive models KW - time series analysis KW - codifference Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab3366 SN - 1367-2630 VL - 21 PB - Deutsche Physikalische Gesellschaft ; IOP, Institute of Physics CY - Bad Honnef und London ER - TY - THES A1 - Thater, Sabine T1 - The interplay between supermassive black holes and their host galaxies T1 - Das Zusammenspiel zwischen supermassereichen Schwarzen Löchern und ihren Muttergalaxien N2 - Supermassive black holes reside in the hearts of almost all massive galaxies. Their evolutionary path seems to be strongly linked to the evolution of their host galaxies, as implied by several empirical relations between the black hole mass (M BH ) and different host galaxy properties. The physical driver of this co-evolution is, however, still not understood. More mass measurements over homogeneous samples and a detailed understanding of systematic uncertainties are required to fathom the origin of the scaling relations. In this thesis, I present the mass estimations of supermassive black holes in the nuclei of one late-type and thirteen early-type galaxies. Our SMASHING sample extends from the intermediate to the massive galaxy mass regime and was selected to fill in gaps in number of galaxies along the scaling relations. All galaxies were observed at high spatial resolution, making use of the adaptive-optics mode of integral field unit (IFU) instruments on state-of-the-art telescopes (SINFONI, NIFS, MUSE). I extracted the stellar kinematics from these observations and constructed dynamical Jeans and Schwarzschild models to estimate the mass of the central black holes robustly. My new mass estimates increase the number of early-type galaxies with measured black hole masses by 15%. The seven measured galaxies with nuclear light deficits (’cores’) augment the sample of cored galaxies with measured black holes by 40%. Next to determining massive black hole masses, evaluating the accuracy of black hole masses is crucial for understanding the intrinsic scatter of the black hole- host galaxy scaling relations. I tested various sources of systematic uncertainty on my derived mass estimates. The M BH estimate of the single late-type galaxy of the sample yielded an upper limit, which I could constrain very robustly. I tested the effects of dust, mass-to-light ratio (M/L) variation, and dark matter on my measured M BH . Based on these tests, the typically assumed constant M/L ratio can be an adequate assumption to account for the small amounts of dark matter in the center of that galaxy. I also tested the effect of a variable M/L variation on the M BH measurement on a second galaxy. By considering stellar M/L variations in the dynamical modeling, the measured M BH decreased by 30%. In the future, this test should be performed on additional galaxies to learn how an as constant assumed M/L flaws the estimated black hole masses. Based on our upper limit mass measurement, I confirm previous suggestions that resolving the predicted BH sphere-of-influence is not a strict condition to measure black hole masses. Instead, it is only a rough guide for the detection of the black hole if high-quality, and high signal-to-noise IFU data are used for the measurement. About half of our sample consists of massive early-type galaxies which show nuclear surface brightness cores and signs of triaxiality. While these types of galaxies are typically modeled with axisymmetric modeling methods, the effects on M BH are not well studied yet. The massive galaxies of our presented galaxy sample are well suited to test the effect of different stellar dynamical models on the measured black hole mass in evidently triaxial galaxies. I have compared spherical Jeans and axisymmetric Schwarzschild models and will add triaxial Schwarzschild models to this comparison in the future. The constructed Jeans and Schwarzschild models mostly disagree with each other and cannot reproduce many of the triaxial features of the galaxies (e.g., nuclear sub-components, prolate rotation). The consequence of the axisymmetric-triaxial assumption on the accuracy of M BH and its impact on the black hole - host galaxy relation needs to be carefully examined in the future. In the sample of galaxies with published M BH , we find measurements based on different dynamical tracers, requiring different observations, assumptions, and methods. Crucially, different tracers do not always give consistent results. I have used two independent tracers (cold molecular gas and stars) to estimate M BH in a regular galaxy of our sample. While the two estimates are consistent within their errors, the stellar-based measurement is twice as high as the gas-based. Similar trends have also been found in the literature. Therefore, a rigorous test of the systematics associated with the different modeling methods is required in the future. I caution to take the effects of different tracers (and methods) into account when discussing the scaling relations. I conclude this thesis by comparing my galaxy sample with the compilation of galaxies with measured black holes from the literature, also adding six SMASHING galaxies, which were published outside of this thesis. None of the SMASHING galaxies deviates significantly from the literature measurements. Their inclusion to the published early-type galaxies causes a change towards a shallower slope for the M BH - effective velocity dispersion relation, which is mainly driven by the massive galaxies of our sample. More unbiased and homogenous measurements are needed in the future to determine the shape of the relation and understand its physical origin. N2 - Supermassereiche schwarze Löcher befinden sich in den Herzen von fast allen massiven Galaxien. Ihr evolutionärer Werdegang scheint stark mit dem Wachstum ihrer Muttergalaxien in Verbindung zu stehen, wie mehrere empirische Beziehungen zwischen der Masse der schwarzen Löcher (M BH ) und verschiedenen Eigenschaften der Muttergalaxien andeuten. Der physikalische Ursprung dieser Koevolution ist jedoch immer noch nicht verstanden. Weitere Massenmessungen über homogene Galaxienproben und ein detailliertes Verständnis der systematischen Unsicherheiten sind erforderlich, um den Ursprung dieser Skalierungsbeziehungen zu ergründen. In dieser Arbeit präsentiere ich die Massenabschätzungen von Supermassereichen Schwarzen Löchern der Zentren einer Spiral- und dreizehn elliptischer und linsenförmiger Galaxien. Meine SMASHING-Probe erstreckt sich vom mittleren bis zum hohen Galaxienmassenbereich und wurde ausgewählt, um Lücken entlang der Skalierungsbeziehungen zu schließen. Alle Galaxien wurden mit hoher räumlicher Auflösung beobachtet, wobei der adaptivoptische Modus von Integralfeldspektrographen (IFU) modernster Teleskope (SINFONI, NIFS, MUSE) verwendet wurde. Aus diesen Beobachtungen habe ich die Sternenkinematik extrahiert und dynamische Jeans- und Schwarzschildmodelle konstruiert, um die Masse der zentralen Schwarzen Löcher robust zu bestimmen. Meine neuen Massenschätzungen erhöhen die Anzahl elliptischer Galaxien mit vermessenen Schwarzen Löchern um 15%. Die sieben vermessenen Galaxien mit inneren Lichtdefiziten ("Cores") ergänzen die Probe der Core-Galaxien mit gemessenen schwarzen Löchern um 40%. Neben der Bestimmung ist die Beurteilung der Genauigkeit von Schwarzlochmassen entscheidend für das Verständnis der intrinsischen Streuung der Beziehungen zwischen schwarzem Loch und Muttergalaxie. Ich habe meine abgeleiteten Massenabschätzungen auf verschiedene systematische Fehlerquellen getestet. Dabei habe ich Bezug genommen auf die Auswirkungen von Staub, Variation des Masse-Licht-Verhältnisses (M/L), Dunkler Materie, verschiedener dynamischer Modelle und verschiedener dynamischer Tracer. Die Ergebnisse präsentiere ich in dieser Arbeit. Ich schließe diese Arbeit, indem ich meine Galaxienprobe mit der den in der Forschungsliteratur zusammengestellten Galaxien mit bereits vermessenen Schwarzen Löchern vergleiche und auch sechs SMASHING-Galaxien hinzufüge, die außerhalb dieser Arbeit veröffentlicht wurden. Keine der SMASHING-Galaxien weicht signifikant von den veröffentlichten Messungen ab. Eine gemeinsame Analyse meiner Messungen und der veröffentlichten elliptischen Galaxien ergibt eine Abflachung der Steigung für die M BH - effektive Geschwindigkeitsdispersionsbeziehung, die hauptsächlich von den massiven Galaxien meiner Probe bewirkt wird. In Zukunft sind unvoreingenommene und homogenere Messungen erforderlich, um die Form der Skalierungsbeziehung zu bestimmen und ihren physikalischen Ursprung zu verstehen. KW - supermassive black holes KW - galaxy evolution KW - stellar kinematics KW - galaxy dynamics KW - integral field spectroscopy KW - supermassereiche Schwarze Löcher KW - Galaxienentwicklung KW - stellare Kinematik KW - Galaxiendynamik KW - Integralfieldspektroskopie Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-437570 ER - TY - THES A1 - Wagle, Swapnil T1 - Multi scale modeling of SNARE-mimetic peptides for their applications in membrane fusion Y1 - 2019 ER - TY - GEN A1 - Guggenberger, Tobias A1 - Pagnini, Gianni A1 - Vojta, Thomas A1 - Metzler, Ralf T1 - Fractional Brownian motion in a finite interval BT - correlations effect depletion or accretion zones of particles near boundaries T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - Fractional Brownian motion (FBM) is a Gaussian stochastic process with stationary, long-time correlated increments and is frequently used to model anomalous diffusion processes. We study numerically FBM confined to a finite interval with reflecting boundary conditions. The probability density function of this reflected FBM at long times converges to a stationary distribution showing distinct deviations from the fully flat distribution of amplitude 1/L in an interval of length L found for reflected normal Brownian motion. While for superdiffusion, corresponding to a mean squared displacement (MSD) 〈X² (t)〉 ⋍ tᵅ with 1 < α < 2, the probability density function is lowered in the centre of the interval and rises towards the boundaries, for subdiffusion (0 < α < 1) this behaviour is reversed and the particle density is depleted close to the boundaries. The MSD in these cases at long times converges to a stationary value, which is, remarkably, monotonically increasing with the anomalous diffusion exponent α. Our a priori surprising results may have interesting consequences for the application of FBM for processes such as molecule or tracer diffusion in the confines of living biological cells or organelles, or other viscoelastic environments such as dense liquids in microfluidic chambers. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 755 KW - anomalous diffusion KW - fractional Brownian motion KW - reflecting boundary conditions Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-436665 SN - 1866-8372 IS - 755 ER - TY - JOUR A1 - Guggenberger, Tobias A1 - Pagnini, Gianni A1 - Vojta, Thomas A1 - Metzler, Ralf T1 - Fractional Brownian motion in a finite interval BT - correlations effect depletion or accretion zones of particles near boundaries JF - New Journal of Physics N2 - Fractional Brownian motion (FBM) is a Gaussian stochastic process with stationary, long-time correlated increments and is frequently used to model anomalous diffusion processes. We study numerically FBM confined to a finite interval with reflecting boundary conditions. The probability density function of this reflected FBM at long times converges to a stationary distribution showing distinct deviations from the fully flat distribution of amplitude 1/L in an interval of length L found for reflected normal Brownian motion. While for superdiffusion, corresponding to a mean squared displacement (MSD) 〈X² (t)〉 ⋍ tᵅ with 1 < α < 2, the probability density function is lowered in the centre of the interval and rises towards the boundaries, for subdiffusion (0 < α < 1) this behaviour is reversed and the particle density is depleted close to the boundaries. The MSD in these cases at long times converges to a stationary value, which is, remarkably, monotonically increasing with the anomalous diffusion exponent α. Our a priori surprising results may have interesting consequences for the application of FBM for processes such as molecule or tracer diffusion in the confines of living biological cells or organelles, or other viscoelastic environments such as dense liquids in microfluidic chambers. KW - anomalous diffusion KW - fractional Brownian motion KW - reflecting boundary conditions Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab075f SN - 1367-2630 VL - 21 PB - Deutsche Physikalische Gesellschaft ; IOP, Institute of Physics CY - Bad Honnef und London ER - TY - GEN A1 - Sposini, Vittoria A1 - Metzler, Ralf A1 - Oshanin, Gleb T1 - Single-trajectory spectral analysis of scaled Brownian motion T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - Astandard approach to study time-dependent stochastic processes is the power spectral density (PSD), an ensemble-averaged property defined as the Fourier transform of the autocorrelation function of the process in the asymptotic limit of long observation times, T → ∞. In many experimental situations one is able to garner only relatively few stochastic time series of finite T, such that practically neither an ensemble average nor the asymptotic limit T → ∞ can be achieved. To accommodate for a meaningful analysis of such finite-length data we here develop the framework of single-trajectory spectral analysis for one of the standard models of anomalous diffusion, scaled Brownian motion.Wedemonstrate that the frequency dependence of the single-trajectory PSD is exactly the same as for standard Brownian motion, which may lead one to the erroneous conclusion that the observed motion is normal-diffusive. However, a distinctive feature is shown to be provided by the explicit dependence on the measurement time T, and this ageing phenomenon can be used to deduce the anomalous diffusion exponent.Wealso compare our results to the single-trajectory PSD behaviour of another standard anomalous diffusion process, fractional Brownian motion, and work out the commonalities and differences. Our results represent an important step in establishing singletrajectory PSDs as an alternative (or complement) to analyses based on the time-averaged mean squared displacement. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 753 KW - diffusion KW - anomalous diffusion KW - power spectral analysis KW - single trajectory analysis Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-436522 SN - 1866-8372 IS - 753 ER - TY - JOUR A1 - Sposini, Vittoria A1 - Metzler, Ralf A1 - Oshanin, Gleb T1 - Single-trajectory spectral analysis of scaled Brownian motion JF - New Journal of Physics N2 - Astandard approach to study time-dependent stochastic processes is the power spectral density (PSD), an ensemble-averaged property defined as the Fourier transform of the autocorrelation function of the process in the asymptotic limit of long observation times, T → ∞. In many experimental situations one is able to garner only relatively few stochastic time series of finite T, such that practically neither an ensemble average nor the asymptotic limit T → ∞ can be achieved. To accommodate for a meaningful analysis of such finite-length data we here develop the framework of single-trajectory spectral analysis for one of the standard models of anomalous diffusion, scaled Brownian motion.Wedemonstrate that the frequency dependence of the single-trajectory PSD is exactly the same as for standard Brownian motion, which may lead one to the erroneous conclusion that the observed motion is normal-diffusive. However, a distinctive feature is shown to be provided by the explicit dependence on the measurement time T, and this ageing phenomenon can be used to deduce the anomalous diffusion exponent.Wealso compare our results to the single-trajectory PSD behaviour of another standard anomalous diffusion process, fractional Brownian motion, and work out the commonalities and differences. Our results represent an important step in establishing singletrajectory PSDs as an alternative (or complement) to analyses based on the time-averaged mean squared displacement. KW - diffusion KW - anomalous diffusion KW - power spectral analysis KW - single trajectory analysis Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab2f52 SN - 1367-2630 VL - 21 PB - Deutsche Physikalische Gesellschaft ; IOP, Institute of Physics CY - Bad Honnef und London ER - TY - GEN A1 - Jelken, Joachim A1 - Santer, Svetlana T1 - Light induced reversible structuring of photosensitive polymer films T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - In this paper we report on photoswitchable polymer surfaces with dynamically and reversibly fluctuating topographies. It is well known that when azobenzene containing polymer films are irradiated with optical interference patterns the film topography changes to form a surface relief grating. In the simplest case, the film shape mimics the intensity distribution and deforms into a wave like, sinusoidal manner with amplitude that may be as large as the film thickness. This process takes place in the glassy state without photo-induced softening. Here we report on an intriguing discovery regarding the formation of reliefs under special illumination conditions. We have developed a novel setup combining the optical part for creating interference patterns, an AFM for in situ acquisition of topography changes and diffraction efficiency signal measurements. In this way we demonstrate that these gratings can be “set in motion” like water waves or dunes in the desert. We achieve this by applying repetitive polarization changes to the incoming interference pattern. Such light responsive surfaces represent the prerequisite for providing practical applications ranging from conveyer or transport systems for adsorbed liquid objects and colloidal particles to generation of adaptive and dynamic optical devices. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 750 KW - surface-relief gratings KW - induced deformation KW - mass-transport KW - azobenzene elastomers KW - thin-films KW - birefringence KW - roughness KW - network KW - erasure Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-436432 SN - 1866-8372 IS - 750 SP - 20295 EP - 20305 ER - TY - JOUR A1 - Jelken, Joachim A1 - Santer, Svetlana T1 - Light induced reversible structuring of photosensitive polymer films JF - RSC Advances N2 - In this paper we report on photoswitchable polymer surfaces with dynamically and reversibly fluctuating topographies. It is well known that when azobenzene containing polymer films are irradiated with optical interference patterns the film topography changes to form a surface relief grating. In the simplest case, the film shape mimics the intensity distribution and deforms into a wave like, sinusoidal manner with amplitude that may be as large as the film thickness. This process takes place in the glassy state without photo-induced softening. Here we report on an intriguing discovery regarding the formation of reliefs under special illumination conditions. We have developed a novel setup combining the optical part for creating interference patterns, an AFM for in situ acquisition of topography changes and diffraction efficiency signal measurements. In this way we demonstrate that these gratings can be “set in motion” like water waves or dunes in the desert. We achieve this by applying repetitive polarization changes to the incoming interference pattern. Such light responsive surfaces represent the prerequisite for providing practical applications ranging from conveyer or transport systems for adsorbed liquid objects and colloidal particles to generation of adaptive and dynamic optical devices. KW - surface-relief gratings KW - induced deformation KW - mass-transport KW - azobenzene elastomers KW - thin-films KW - birefringence KW - roughness KW - network KW - erasure Y1 - 2019 U6 - https://doi.org/10.1039/C9RA02571E SN - 2046-2069 VL - 9 IS - 35 SP - 20295 EP - 20305 PB - RSC Publishing CY - London ER - TY - THES A1 - Bachmann, Felix T1 - Non-linearity of magnetic micropropellers BT - chances and challenges of complex dynamics at the microscale Y1 - 2019 ER - TY - THES A1 - Ramachandran, Varsha T1 - Massive star evolution, star formation, and feedback at low metallicity T1 - Massive Sternentwicklung, Sternentstehung, und das Feedback bei niedriger Metallizität BT - quantitative spectroscopy of OB stars in the Magellanic Clouds N2 - The goal of this thesis is to broaden the empirical basis for a better, comprehensive understanding of massive star evolution, star formation and feedback at low metallicity. Low metallicity massive stars are a key to understand the early universe. Quantitative information on metal-poor massive stars was sparse before. The quantitative spectroscopic studies of massive star populations associated with large-scale ISM structures were not performed at low metallicity before, but are important to investigate star-formation histories and feedback in detail. Much of this work relies on spectroscopic observations with VLT-FLAMES of ~500 OB stars in the Magellanic Clouds. When available, the optical spectroscopy was complemented by UV spectra from the HST, IUE, and FUSE archives. The two representative young stellar populations that have been studied are associated with the superbubble N 206 in the Large Magellanic Cloud (LMC) and with the supergiant shell SMC-SGS 1 in the Wing of the Small Magellanic Cloud (SMC), respectively. We performed spectroscopic analyses of the massive stars using the nonLTE Potsdam Wolf-Rayet (PoWR) model atmosphere code. We estimated the stellar, wind, and feedback parameters of the individual massive stars and established their statistical distributions. The mass-loss rates of N206 OB stars are consistent with theoretical expectations for LMC metallicity. The most massive and youngest stars show nitrogen enrichment at their surface and are found to be slower rotators than the rest of the sample. The N 206 complex has undergone star formation episodes since more than 30 Myr, with a current star formation rate higher than average in the LMC. The spatial age distribution of stars across the complex possibly indicates triggered star formation due to the expansion of the superbubble. Three very massive, young Of stars in the region dominate the ionizing and mechanical feedback among hundreds of other OB stars in the sample. The current stellar wind feedback rate from the two WR stars in the complex is comparable to that released by the whole OB sample. We see only a minor fraction of this stellar wind feedback converted into X-ray emission. In this LMC complex, stellar winds and supernovae equally contribute to the total energy feedback, which eventually powered the central superbubble. However, the total energy input accumulated over the time scale of the superbubble significantly exceeds the observed energy content of the complex. The lack of energy along with the morphology of the complex suggests a leakage of hot gas from the superbubble. With a detailed spectroscopic study of massive stars in SMC-SGS 1, we provide the stellar and wind parameters of a large sample of OB stars at low metallicity, including those in the lower mass-range. The stellar rotation velocities show a broad, tentatively bimodal distribution, with Be stars being among the fastest. A few very luminous O stars are found close to the main sequence, while all other, slightly evolved stars obey a strict luminosity limit. Considering additional massive stars in evolved stages, with published parameters and located all over the SMC, essentially confirms this picture. The comparison with single-star evolutionary tracks suggests a dichotomy in the fate of massive stars in the SMC. Only stars with an initial mass below 30 solar masses seem to evolve from the main sequence to the cool side of the HRD to become a red supergiant and to explode as type II-P supernova. In contrast, more massive stars appear to stay always hot and might evolve quasi chemically homogeneously, finally collapsing to relatively massive black holes. However, we find no indication that chemical mixing is correlated with rapid rotation. We measured the key parameters of stellar feedback and established the links between the rates of star formation and supernovae. Our study demonstrates that in metal-poor environments stellar feedback is dominated by core-collapse supernovae in combination with winds and ionizing radiation supplied by a few of the most massive stars. We found indications of the stochastic mode of star formation, where the resulting stellar population is fully capable of producing large-scale structures such as the supergiant shell SMC-SGS 1 in the Wing. The low level of feedback in metal-poor stellar populations allows star formation episodes to persist over long timescales. Our study showcases the importance of quantitative spectroscopy of massive stars with adequate stellar-atmosphere models in order to understand star-formation, evolution, and feedback. The stellar population analyses in the LMC and SMC make us understand that massive stars and their impact can be very different depending on their environment. Obviously, due to their different metallicity, the massive stars in the LMC and the SMC follow different evolutionary paths. Their winds differ significantly, and the key feedback agents are different. As a consequence, the star formation can proceed in different modes. N2 - Massereiche Sterne, also Sterne, die ihre Entwicklung mit mehr als acht Sonnenmassen starten, spielen die Hauptrolle in der chemischen Entwicklung des Universums. Darüberhinaus formen sie das sie umgebende interstellare Medium, aus dem sie entstanden sind, durch ihre ionisierende Strahlung und ihre starken Massenausflüsse in Form von Sternwinden und Supernovaexplosionen, das sogenannte Feedback. Diese Arbeit verbreitert die empirische Basis für ein besseres Verständnis der Entwicklung, Entstehung und des Feedbacks massereicher Sterne bei niedriger Metallizität, wie sie auch im frühen Universum herrschte, wesentlich. Hierfür wurden die Daten von zwei großen spektroskopischen Beobachtungskampagnen in der Großen (LMC) und in der Kleinen Magellanschen Wolke (SMC) - beides Galaxien mit erniedrigter Metallizität - mittels des Non-LTE Potsdam Wolf-Rayet (PoWR) Model Atmosphere Codes quantitativ analysiert, um wesentliche Stern-, Wind- und Feedbackparameter sowie ihre statistische Verteilung zu bestimmen und damit ein globales Bild der massereichen Sterne und ihrer Wechselwirkung mit der Umgebung zu erhalten. Diese Analysen stützen sich hauptsächlich auf Spektren aus dem optischen Bereich, die mit dem Fibre Large Array Multi Element Spectrograph (FLAMES) am Very Large Telescope (VLT) von ~ 500 OBSternen in den Magellanschen Wolken aufgenommen worden, ergänzt durch UV-Spektren aus den Archiven verschiedener UV-Satelliten. Die zwei repräsentativen jungen Sternpopulationen, die untersucht wurden, gehören zur Superbubble N206 in der LMC beziehungsweise zur Supergiant Shell SMC-SGS 1 im Wing der SMC. Die analysierte Stichprobe des N206-Komplexes umfasst alle heißen massereichen Sterne vom Typ OB, Of, und Wolf-Rayet, wobei letztere weit entwickelt und durch starke Sternwinde gekennzeichnet sind. Auf Basis unsere Analysen fanden wir heraus, dass der Komplex seit 30 Mio. Jahren mehrere Sternentstehungsepisoden durchlief. Die räumliche Altersverteilung dieser Sterne über den Komplex weist möglicherweise auf getriggerte Sternentstehung infolge der Ausdehnung der Superbubble hin. Drei sehr massereiche, junge Of-Sterne in dieser Region dominieren das ionisierende und mechanische Feedback unter hunderten von anderen OBSternen in der Region. Die SMC hat eine noch niedrigere Metallizität als die LMC, was sich u.a. auch in der Sternentwicklung niederschlagen sollte. Daher wurde mittels der Daten der Spektralanalysen der Supergiant Shell SMC-SGS 1 in der SMC zusammen mit weiteren Daten aus der Literatur das am dichtesten besiedelte Hertzsprung-Russell-Diagramm der massereichen Sterne in der SMC erstellt. Der Vergleich mit Sternentwicklungsrechnungen suggeriert eine Zweiteilung der Entwicklungswege massereicher Sterne in der SMC. Dabei scheint die gemessene Rotation der Sterne überraschenderweise keinen großen Einfluss zu haben. Wir vermuten daher, dass die Masse und Metallizität der Sterne zusammen hauptverantwortlich für die beobachtete Zweiteilung sind. Desweiteren konnte erstmalig auf einer breiten Datenbasis aufbauend die Korrelation zwischen Metallizität und Stärke von OB-Sternwinden etabliert werden, allerdings sind die ermittelten Windstärken weit schwächer als vorhergesagt (Weak-Wind-Problem) und in Sternentwicklungsrechnungen verwendet. Die Alter und räumliche Verteilung von massereichen Sternen zeigen, dass Sternentstehung seit über 100 Mio. Jahren in der ruhigen Region niedriger Dichte in der SMC eher stochastisch als sequenziell voranschreitet und höher ist als von Messungen diffuser Hα-Emission abgeleitet wurde. Das Feedback in dieser Region wird aufgrund der schwachen Sternwinde durch Supernovae bestimmt, während die Ionization der gesamten Region durch einen einzigen sehr heißen und leuchtkräftigen Wolf-Rayet-Stern dominiert wird. Die niedrige Feedbackrate in metallarmen Sternpopulationen scheint für die Größe und das Überleben von Molekülwolken förderlich zu sein, sodass Sternentstehungsepisoden über einen längeren Zeitraum ablaufen. Solch ausgedehnte Sternentstehung kann dazu führen, dass es eine fortwährende Quelle von ionisierenden Photonen gibt, welche in das zirkumgalaktische Medium durch Löcher oder Kanäle entweichen können, die durch Supernovae erzeugt worden. Diese Studie regt an, dass Sternentstehungsregionen mit langer Geschichte ihre Spuren im umgebenden ISM auch bei niedriger Metallizität hinterlassen werden. Die zukünftigen großräumigen Spektroskopiestudien von weiter entfernten Galaxien mit noch geringeren Metallizitäten können weitere Einsichten in unser derzeitiges Verständnis von massereichen Sternen bringen. KW - massive stars KW - stellar feedback KW - spectroscopy KW - stellar evolution KW - star formation KW - massive Sterne KW - Sternfeedback KW - Spektroskopie KW - Sternentwicklung KW - Sternentstehung Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-432455 ER - TY - THES A1 - Sablowski, Daniel T1 - Spectroscopic analysis of the benchmark system Alpha Aurigae T1 - Spektroskopische Analysen des Vergleichssystems alpha Aurigae N2 - Binaries play an important role in observational and theoretical astrophysics. Since the mass and the chemical composition are key ingredients for stellar evolution, high-resolution spectroscopy is an important and necessary tool to derive those parameters to high confidence in binaries. This involves carefully measured orbital motion by the determination of radial velocity (RV) shifts and sophisticated techniques to derive the abundances of elements within the stellar atmosphere. A technique superior to conventional cross-correlation methods to determine RV shifts in known as spectral disentangling. Hence, a major task of this thesis was the design of a sophisticated software package for this approach. In order to investigate secondary effects, such as flux and line-profile variations, imprinting changes on the spectrum the behavior of spectral disentangling on such variability is a key to understand the derived values, to improve them, and to get information about the variability itself. Therefore, the spectral disentangling code presented in this thesis and available to the community combines multiple advantages: separation of the spectra for detailed chemical analysis, derivation of orbital elements, derivation of individual RVs in order to investigate distorted systems (either by third body interaction or relativistic effects), the suppression of telluric contaminations, the derivation of variability, and the possibility to apply the technique to eclipsing binaries (important for orbital inclination) or in general to systems that undergo flux-variations. This code in combination with the spectral synthesis codes MOOG and SME was used in order to derive the carbon 12C/13C isotope ratio (CIR) of the benchmark binary Capella. The observational result will be set into context with theoretical evolution by the use of MESA models and resolves the discrepancy of theory and observations existing since the first measurement of Capella's CIR in 1976. The spectral disentangling code has been made available to the community and its applicability to completely different behaving systems, Wolf-Rayet stars, have also been investigated and resulted in a published article. Additionally, since this technique relies strongly on data quality, continues development of scientific instruments to achieve best observational data is of great importance in observational astrophysics. That is the reason why there has also been effort in astronomical instrumentation during the work on this thesis. N2 - Doppelsterne spielen eine wichtige Rolle in der beobachtenden und theoretischen Astrophysik. Die Massen und die chemische Zusammensetzung der Sterne sind dabei ausschlaggebende Parameter. Die wichtige und notwendige Methode um diese zu bestimmen ist hochaufgelöste Spektroskopie. Dies beinhaltet eine penible Bestimmung der orbitalen Bewegung durch die Vermessung von Radialgeschwindigkeitsverschiebungen (RV) und fortgeschrittene Techniken zur Bestimmung der Häufigkeiten der in der Sternatmosphäre vorhandenen Elemente. Gegenüber der konventionellen Kreuzkorrelation zur Bestimmung der RV-Verschiebungen, gilt die Methode des sogenannten 'spectral disentanglings' als überlegen. Daher bestand ein Großteil der vorliegenden Arbeit darin, eine solche Methode in einem weiterentwickelten Softwarepacket zu realisieren. Um sekundäre Effekte zu verstehen, welche zu weiteren Änderungen im Spektrum führen, also insbesondere solche wie Fluss- und Linienprofilvariationen, ist es von zentraler Bedeutung das Verhalten des spectral disentangling durch solche Variabilitäten zu verstehen, sodass die ermittelten Größen besser interpretiert und verbessert, sowie Informationen über die Variabilität selbst abgeleitet werden können. Daher vereint der in dieser Arbeit vorgestellte und der Allgemeinheit offen stehende Algorithmus für das spectral disentangling mehrere Vorteile: Separation der Spektren für detaillierte chemische Analysen, Ableitung der orbitalen Bahnelemente, Ableitung der einzelnen RV-Verschiebungen um auch gestörte Systeme (z.B. durch einen dritten Körper oder relativistische Effekte) analysieren zu können, die Reduktion des Einflusses tellurischer Kontamination, Ableitung der Variabilität und die Möglichkeit der Anwendung auf Bedeckungsveränderliche (wichtig zur Bestimmung der Inklination) bzw. allgemeiner auf Systeme mit Flussvariationen. Der vorgestellte Algorithmus wurde zusammen mit MOOG und SME zur Erzeugung synthetischer Spektren verwendet um das Kohlenstoff-12C/13C Isotopen-Verhältnis (KIV) des Referenzsystems Capella zu bestimmen. Dieses Ergebnis aus Beobachtungen wird in Kontext zur theoretischen Entwicklung durch Verwendung von MESA Modellen gesetzt und löst die Unstimmigkeit zwischen Beobachtung und Theorie die bereits seit der ersten Messung des KIV von Kapella von 1976 existiert. Der Algorithmus für das spectral disentangling ist der Allgemeinheit zugänglich gemacht und wurde auf vollkommen anders verhaltende Objekte, den Wolf-Rayet-Sternen, angewendet, was in einer publizierten Arbeit resultierte. Da die Methode stark von der Qualität der Beobachtungsdaten abhängt, ist eine kontinuierliche Weiterentwicklung der wissenschaftlichen Messtechnik der beobachtenden Astrophysik sehr wichtig um die bestmöglichsten Beobachtungsdaten gewinnen zu können. Daher wurden auch große Anstrengungen in der astronomischen Instrumentierung während dieser Arbeit unternommen. KW - Stellar physics KW - Stellar evolution KW - spectroscopy KW - instrumentation KW - carbon-isotope-ratio KW - Capella KW - Stellarphysik KW - Sternentwicklung KW - Spektroskopie KW - Instrumentierung KW - Kohlenstoff-Isotopen-Verhältnis KW - Kapella Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-432396 ER - TY - THES A1 - Haase, Nadin T1 - The nascent peptide chain in the ribosomal exit tunnel Y1 - 2019 ER - TY - THES A1 - Peter, Franziska T1 - Transition to synchrony in finite Kuramoto ensembles T1 - Synchronisationsübergang in endlichen Kuramoto-Ensembles N2 - Synchronisation – die Annäherung der Rhythmen gekoppelter selbst oszillierender Systeme – ist ein faszinierendes dynamisches Phänomen, das in vielen biologischen, sozialen und technischen Systemen auftritt. Die vorliegende Arbeit befasst sich mit Synchronisation in endlichen Ensembles schwach gekoppelter selbst-erhaltender Oszillatoren mit unterschiedlichen natürlichen Frequenzen. Das Standardmodell für dieses kollektive Phänomen ist das Kuramoto-Modell – unter anderem aufgrund seiner Lösbarkeit im thermodynamischen Limes unendlich vieler Oszillatoren. Ähnlich einem thermodynamischen Phasenübergang zeigt im Fall unendlich vieler Oszillatoren ein Ordnungsparameter den Übergang von Inkohärenz zu einem partiell synchronen Zustand an, in dem ein Teil der Oszillatoren mit einer gemeinsamen Frequenz rotiert. Im endlichen Fall treten Fluktuationen auf. In dieser Arbeit betrachten wir den bisher wenig beachteten Fall von bis zu wenigen hundert Oszillatoren, unter denen vergleichbar starke Fluktuationen auftreten, bei denen aber ein Vergleich zu Frequenzverteilungen im unendlichen Fall möglich ist. Zunächst definieren wir einen alternativen Ordnungsparameter zur Feststellung einer kollektiven Mode im endlichen Kuramoto-Modell. Dann prüfen wir die Abhängigkeit des Synchronisationsgrades und der mittleren Rotationsfrequenz der kollektiven Mode von Eigenschaften der natürlichen Frequenzverteilung für verschiedene Kopplungsstärken. Wir stellen dabei zunächst numerisch fest, dass der Synchronisationsgrad stark von der Form der Verteilung (gemessen durch die Kurtosis) und die Rotationsfrequenz der kollektiven Mode stark von der Asymmetrie der Verteilung (gemessen durch die Schiefe) der natürlichen Frequenzen abhängt. Beides können wir im thermodynamischen Limes analytisch verifizieren. Mit diesen Ergebnissen können wir Erkenntnisse anderer Autoren besser verstehen und verallgemeinern. Etwas abseits des roten Fadens dieser Arbeit finden wir außerdem einen analytischen Ausdruck für die Volumenkontraktion im Phasenraum. Der zweite Teil der Arbeit konzentriert sich auf den ordnenden Effekt von Fluktuationen, die durch die Endlichkeit des Systems zustande kommen. Im unendlichen Modell sind die Oszillatoren eindeutig in kohärent und inkohärent und damit in geordnet und ungeordnet getrennt. Im endlichen Fall können die auftretenden Fluktuationen zusätzliche Ordnung unter den asynchronen Oszillatoren erzeugen. Das grundlegende Prinzip, die rauschinduzierte Synchronisation, ist aus einer Reihe von Publikationen bekannt. Unter den gekoppelten Oszillatoren nähern sich die Phasen aufgrund der Fluktuationen des Ordnungsparameters an, wie wir einerseits direkt numerisch zeigen und andererseits mit einem Synchronisationsmaß aus der gerichteten Statistik zwischen Paaren passiver Oszillatoren nachweisen. Wir bestimmen die Abhängigkeit dieses Synchronisationsmaßes vom Verhältnis von paarweiser natürlicher Frequenzdifferenz zur Varianz der Fluktuationen. Dabei finden wir eine gute Übereinstimmung mit einem einfachen analytischen Modell, in welchem wir die deterministischen Fluktuationen des Ordnungsparameters durch weißes Rauschen ersetzen. N2 - Synchronization – the adjustment of rhythms among coupled self-oscillatory systems – is a fascinating dynamical phenomenon found in many biological, social, and technical systems. The present thesis deals with synchronization in finite ensembles of weakly coupled self-sustained oscillators with distributed frequencies. The standard model for the description of this collective phenomenon is the Kuramoto model – partly due to its analytical tractability in the thermodynamic limit of infinitely many oscillators. Similar to a phase transition in the thermodynamic limit, an order parameter indicates the transition from incoherence to a partially synchronized state. In the latter, a part of the oscillators rotates at a common frequency. In the finite case, fluctuations occur, originating from the quenched noise of the finite natural frequency sample. We study intermediate ensembles of a few hundred oscillators in which fluctuations are comparably strong but which also allow for a comparison to frequency distributions in the infinite limit. First, we define an alternative order parameter for the indication of a collective mode in the finite case. Then we test the dependence of the degree of synchronization and the mean rotation frequency of the collective mode on different characteristics for different coupling strengths. We find, first numerically, that the degree of synchronization depends strongly on the form (quantified by kurtosis) of the natural frequency sample and the rotation frequency of the collective mode depends on the asymmetry (quantified by skewness) of the sample. Both findings are verified in the infinite limit. With these findings, we better understand and generalize observations of other authors. A bit aside of the general line of thoughts, we find an analytical expression for the volume contraction in phase space. The second part of this thesis concentrates on an ordering effect of the finite-size fluctuations. In the infinite limit, the oscillators are separated into coherent and incoherent thus ordered and disordered oscillators. In finite ensembles, finite-size fluctuations can generate additional order among the asynchronous oscillators. The basic principle – noise-induced synchronization – is known from several recent papers. Among coupled oscillators, phases are pushed together by the order parameter fluctuations, as we on the one hand show directly and on the other hand quantify with a synchronization measure from directed statistics between pairs of passive oscillators. We determine the dependence of this synchronization measure from the ratio of pairwise natural frequency difference and variance of the order parameter fluctuations. We find a good agreement with a simple analytical model, in which we replace the deterministic fluctuations of the order parameter by white noise. KW - synchronization KW - Kuramoto model KW - finite size KW - phase transition KW - dynamical systems KW - networks KW - Synchronisation KW - Kuramoto-Modell KW - endliche Ensembles KW - Phasenübergang KW - dynamische Systeme KW - Netzwerke Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-429168 ER - TY - THES A1 - Kurpiers, Jona T1 - Probing the pathways of free charge generation and recombination in organic solar cells T1 - Pfade der Generierung und Rekombination freier Ladungsträger in organischen Solarzellen BT - the role of excess energy and dispersive effects BT - die Rolle von Überschussenergie und dispersiven Effekten N2 - Organic semiconductors are a promising class of materials. Their special properties are the particularly good absorption, low weight and easy processing into thin films. Therefore, intense research has been devoted to the realization of thin film organic solar cells (OPVs). Because of the low dielectric constant of organic semiconductors, primary excitations (excitons) are strongly bound and a type II heterojunction needs to be introduced to split these excitations into free charges. Therefore, most organic solar cells consist of at least an electron donor and electron acceptor material. For such donor acceptor systems mainly three states are relevant; the photoexcited exciton on the donor or acceptor material, the charge transfer state at the donor-acceptor interface and the charge separated state of a free electron and hole. The interplay between these states significantly determines the efficiency of organic solar cells. Due to the high absorption and the low charge carrier mobilities, the active layers are usually thin but also, exciton dissociation and free charge formation proceeds rapidely, which makes the study of carrier dynamics highly challenging. Therefore, the focus of this work was first to install new experimental setups for the investigation of the charge carrier dynamics in complete devices with superior sensitivity and time resolution and, second, to apply these methods to prototypical photovoltaic materials to address specific questions in the field of organic and hybrid photovoltaics. Regarding the first goal, a new setup combining transient absorption spectroscopy (TAS) and time delayed collection field (TDCF) was designed and installed in Potsdam. An important part of this work concerned the improvement of the electronic components with respect to time resolution and sensitivity. To this end, a highly sensitive amplifier for driving and detecting the device response in TDCF was developed. This system was then applied to selected organic and hybrid model systems with a particular focus on the understanding of the loss mechanisms that limit the fill factor and short circuit current of organic solar cells. The first model system was a hybrid photovoltaic material comprising inorganic quantum dots decorated with organic ligands. Measurements with TDCF revealed fast free carrier recombination, in part assisted by traps, while bias-assisted charge extraction measurements showed high mobility. The measured parameters then served as input for a successful description of the device performance with an analytical model. With a further improvement of the instrumentation, a second topic was the detailed analysis of non-geminate recombination in a disordered polymer:fullerene blend where an important question was the effect of disorder on the carrier dynamics. The measurements revealed that early time highly mobile charges undergo fast non-geminate recombination at the contacts, causing an apparent field dependence of free charge generation in TDCF experiments if not conducted properly. On the other hand, recombination the later time scale was determined by dispersive recombination in the bulk of the active layer, showing the characteristics of carrier dynamics in an exponential density of state distribution. Importantly, the comparison with steady state recombination data suggested a very weak impact of non-thermalized carriers on the recombination properties of the solar cells under application relevant illumination conditions. Finally, temperature and field dependent studies of free charge generation were performed on three donor-acceptor combinations, with two donor polymers of the same material family blended with two different fullerene acceptor molecules. These particular material combinations were chosen to analyze the influence of the energetic and morphology of the blend on the efficiency of charge generation. To this end, activation energies for photocurrent generation were accurately determined for a wide range of excitation energies. The results prove that the formation of free charge is via thermalized charge transfer states and does not involve hot exciton splitting. Surprisingly, activation energies were of the order of thermal energy at room temperature. This led to the important conclusion that organic solar cells perform well not because of predominate high energy pathways but because the thermalized CT states are weakly bound. In addition, a model is introduced to interconnect the dissociation efficiency of the charge transfer state with its recombination observable with photoluminescence, which rules out a previously proposed two-pool model for free charge formation and recombination. Finally, based on the results, proposals for the further development of organic solar cells are formulated. N2 - Organische Halbleiter sind eine vielversprechende Materialklasse. Ihre besonderen Eigenschaften sind die gute Absorption, das geringe Gewicht und die einfache Verarbeitung zu dünnen Filmen. Daher wird intensiv an der Realisierung organischer Dünnschichtsolarzellen (OPVs) geforscht. Aufgrund der niedrigen Dielektrizitätskonstante organischer Halbleiter sind primäre Anregungen (Exzitonen) jedoch stark gebunden, und es muss ein Typ II-Heteroübergang eingeführt werden, um diese Anregungen in freie Ladungen zu trennen. Daher bestehen die meisten organischen Solarzellen aus mindestens einem Elektronendonator und einem Elektronenakzeptormaterial. Für solche Donator-Akzeptorsysteme sind hauptsächlich drei Zustünde relevant; das Exziton auf dem Donator- oder Akzeptormaterial, der Ladungstransferzustand an der Donator-Akzeptor-Grenzfläche und der ladungsgetrennte Zustand eines freien Elektrons und Lochs. Das Zusammenspiel dieser Zustände bestimmt maßgeblich die Effizienz organischer Solarzellen. Aufgrund der hohen Absorption und der geringen Ladungsträgermobilitäten sind die aktiven Schichten dünn, aber auch die Exzitonendissoziation und die Bildung freier Ladung findet auf kurzen Zeitskalen statt, was die Analyse der Ladungsträgerdynamik erschwert. Im Mittelpunkt dieser Arbeit standen daher zunächst die Installation neuer Versuchsaufbauten zur Untersuchung der Ladungsträgerdynamik in optimierten Solarzellen mit überlegener Empfindlichkeit und Zeitauflösung sowie die Anwendung dieser Methoden auf prototypische photovoltaische Materialien. Im Hinblick auf das erste Ziel wurde ein neuer Aufbau, der optische Methoden wie die zeitaufgelöste Absorptionsspektroskopie (TAS) mit optolektronischen Methoden, wie die zeitaufgelöste Ladungsextraktion (TDCF) kombiniert. Ein wichtiger Teil dieser Arbeit war die Verbesserung der elektronischen Komponenten hinsichtlich der Zeitauflösung und Empfindlichkeit. Zu diesem Zweck wurde ein hochempfindlicher Verstärker zur Ansteuerung und Detektion der Probenantwort in TDCF entwickelt. Dieser Versuchsaufbau wurde im Folgenden auf verschiedene Modellsysteme angewendet, mit besonderem Fokus auf dem Verständnis der Verlustmechanismen, die den Füllfaktor und den Kurzschlussstrom organischer Solarzellen limittieren. Das erste Modellsystem ist ein hybrides Material, das aus anorganischen Quantenpunkten mit organischen Liganden besteht. Messungen mit TDCF ergaben eine schnelle Rekombination freier Ladungsträger, die teilweise durch Fallen unterstützt wurde, während Ladungsextraktionsexperimente unter quasi-konstanter Beleuchtung eine hohe Mobilität zeigten. Mit den gemessenen Parametern konnte die Kennlinie gut mit einem analytischen Modell beschrieben werden. Mit einer weiteren Verbesserung des Aufbaus konnte ein zweites Thema, die detaillierte Analyse der nicht-geminalen Rekombination in einer ungeordneten Polymer-Fulleren-Mischung bearbeitet werden. Die Messungen zeigten, dass hochmobilen Ladungen zu frühen Zeiten eine schnelle, nicht-geminale Rekombination an den Kontakten durchlaufen, was eine scheinbare Feldabhängigkeit der Generierung freier Ladung in TDCF-Experimenten verursachen kann. Andererseits wurde die Rekombination auf längeren Zeitskalen durch dispersive Rekombination in der aktiven Schicht bestimmt, wobei die Ursache der Ladungsträgerdynamik in einer exponentiellen Verteilung der Zustandsdichte liegt. Der Vergleich mit Rekombinationsdaten im stationären Zustand ergab einen sehr schwachen Einfluss nicht-thermalisierter Ladungsträger auf die Rekombinationseigenschaften der Solarzellen unter anwendungsrelevanten Bedingungen. Schließlich wurden temperatur- und feldabhängige Studien zur Erzeugung freier Ladung an drei Donator-Akzeptor-Kombinationen durchgeführt, wobei zwei Donatorpolymere der gleichen Materialfamilie mit zwei verschiedenen Fulleren-Akzeptormolekülen gemischt wurden. Diese besonderen Materialkombinationen wurden ausgewählt, um den Einfluss der Energetik und Morphologie der Mischung auf die Effizienz der Ladungserzeugung zu analysieren. Zu diesem Zweck wurden die Aktivierungsenergien für die Photostromerzeugung für einen weiten Bereich von Anregungsenergien genau bestimmt. Die Ergebnisse beweisen, dass die Bildung freier Ladungen über thermalisierte Ladungstransferzustände erfolgt und keine Aufspaltung mit heißen Exzitonen beinhaltet. Überraschenderweise sind die Aktivierungsenergien vergleichbar mit der thermischen Energie bei Raumtemperatur. Dies führte zu der wichtigen Schlussfolgerung, dass organische Solarzellen nicht aufgrund von hochenergetischen Pfaden gut funktionieren, sondern weil die thermalisierten Ladungstransferzustände schwach gebunden sind. Darüber hinaus wird ein Modell eingeführt, um die Dissoziationseffizienz des Ladungstransferzustands mit seiner mit Photolumineszenz beobachtbaren Rekombination zu verbinden, wodurch ein zuvor vorgeschlagenes Zwei-Pool-Modell für die Bildung und Rekombination von freien Ladungen ausgeschlossen wird. Abschließend werden auf Basis der Ergebnisse Vorschläge zur Weiterentwicklung organischer Solarzellen formuliert. KW - organic solar cells KW - time resolved pump probe spectroscopy Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-429099 ER - TY - THES A1 - Kav, Batuhan T1 - Membrane adhesion mediated via lipid-anchored saccharides T1 - Membranadhäsion durch Lipid-verankerte Saccharide N2 - Membrane adhesion is a fundamental biological process in which membranes are attached to neighboring membranes or surfaces. Membrane adhesion emerges from a complex interplay between the binding of membrane-anchored receptors/ligands and the membrane properties. In this work, we study membrane adhesion mediated by lipid-anchored saccharides using microsecond-long full-atomistic molecular dynamics simulations. Motivated by neutron scattering experiments on membrane adhesion via lipid-anchored saccharides, we investigate the role of LeX, Lac1, and Lac2 saccharides and membrane fluctuations in membrane adhesion. We study the binding of saccharides in three different systems: for saccharides in water, for saccharides anchored to essentially planar membranes at fixed separations, and for saccharides anchored to apposing fluctuating membranes. Our simulations of two saccharides in water indicate that the saccharides engage in weak interactions to form dimers. We find that the binding occurs in a continuum of bound states instead of a certain number of well-defined bound structures, which we term as "diffuse binding". The binding of saccharides anchored to essentially planar membranes strongly depends on separation of the membranes, which is fixed in our simulation system. We show that the binding constants for trans-interactions of two lipid-anchored saccharides monotonically decrease with increasing separation. Saccharides anchored to the same membrane leaflet engage in cis-interactions with binding constants comparable to the trans-binding constants at the smallest membrane separations. The interplay of cis- and trans-binding can be investigated in simulation systems with many lipid-anchored saccharides. For Lac2, our simulation results indicate a positive cooperativity of trans- and cis-binding. In this cooperative binding the trans-binding constant is enhanced by the cis-interactions. For LeX, in contrast, we observe no cooperativity between trans- and cis-binding. In addition, we determine the forces generated by trans-binding of lipid-anchored saccharides in planar membranes from the binding-induced deviations of the lipid-anchors. We find that the forces acting on trans-bound saccharides increase with increasing membrane separation to values of the order of 10 pN. The binding of saccharides anchored to the fluctuating membranes results from an interplay between the binding properties of the lipid-anchored saccharides and membrane fluctuations. Our simulations, which have the same average separation of the membranes as obtained from the neutron scattering experiments, yield a binding constant larger than in planar membranes with the same separation. This result demonstrates that membrane fluctuations play an important role at average membrane separations which are seemingly too large for effective binding. We further show that the probability distribution of the local separation can be well approximated by a Gaussian distribution. We calculate the relative membrane roughness and show that our results are in good agreement with the roughness values reported from the neutron scattering experiments. N2 - Membranadhäsion ist ein fundamentaler biologischer Prozess, bei dem Membranen sich an benachbarte Membranen oder Oberfläche anheften. Membranadhäsion entstammt einem komplexen Zusammenspiel aus Bindungen zwischen Membranverankerten Rezeptor/Ligand-Bindungen und den Membraneigenschaften selbst. In dieser Arbeit untersuchen wir Membranadhäsion vermittelt durch Lipid-verankerte Saccharide mittels Mikrosekunden-langer voll-atomistischer molekular-dynamischer Simulationen. Motiviert durch Neutronen Scattering Experimente von Lipid-verankerten Sacchariden und deren Einfluss auf Membranadhäsion, untersuchen wir die Rolle der Saccharide LeX, Lac1 und Lac2 sowie der Membranfluktuationen in Membranadhäsion. Wir untersuchen die Bindungen der Saccharide in drei verschiedenen Systemen: In Wasser, verankert in quasi-ebenflächigen Membranen bei fixierten Abständen, und verankert in aneinanderliegenden, fluktuierenden Membranen. Unsere Simulationen von zwei Sacchariden in Wasser deuten darauf hin, dass diese Saccharide durch schwache Interaktionen Dimere formen. Anstelle einiger klar definierter Bindungsstrukturen, finden wir ein Kontinuum von gebundenen Zuständen vor, das wir als "diffuse Bindung" bezeichnen. Die Bindungen von Sacchariden in quasi-ebenflächigen Membranen hängt stark vom Abstand zwischen diesen Membranen ab, der in unserem System fest gewählt ist. Wir zeigen, dass die Bundungskonstanten für trans-Interaktionen zweier Lipid-verankerter Saccharide monoton abnimmt mit zunehmendem Abstand. Saccharide verankert auf der selben Membran wechselwirken in cis-Interaktionen, deren Bindungskonstanten denen der trans-Interaktionen bei dem kleinsten gewählten Membranabstand ähneln. Das Zusammenspiel der cis- und trans-Interaktionen kann in Simulationssystemen mit vielen Lipid-verankerten Sacchariden untersucht werden. Für Lac2 deuten unsere Simulationen auf eine Kooperativität zwischen cis- und trans-Interaktionen hin: In diesem kooperativen Bindungsprozess verstärkt die cis-Interkation die trans-Bindunskonstante. Für LeX hingegen stellen wir keine Kooperativität zwischen trans- und cis-Bindung fest. Zusätzlich bestimmen wir die generierten Kräfte, die durch trans-gebundene Lipid-verankerte Saccharide in ebenflächigen Membranen und die resultierende Ablenkung der Lipid-Anker hervorgerufen werden. Wir stellen fest, dass mit gesteigertem Abstand zwischen den Membranen, die auf trans-gebundene Saccharide wirkenden Kräfte auf bis zu 10 pN ansteigen. Die Bindungen von Sacchariden, die in fluktuierenden Membranen verankert sind, resultieren aus einem Zusammenspiel zwischen den Eigenschaften dieser Lipid-verankerten Saccharide und den Membranfluktuationen. Unsere Simulationen, die den Membranabstand aufweisen, der auch in den Neutron Scattering Experimenten ermittelt wurde, resultieren in einer Bindungskonstante, die größer ist als jene in quasi-ebenflächigen Membranen bei dem gleichen Abstand. Dieses Ergebnis demonstriert, dass Membranfluktuationen eine wichtige Rolle spielen bei mittleren Membranabstünden, die sonst scheinbar zu groß sind für effektive Bindungsprozesse. Weiterhin zeigen wir, dass die Wahrscheinlichkeitsverteilung der lokalen Abstünde gut durch eine Gauss-Verteilung approximiert werden kann. Wir berechnen die relative Membranrauigkeit und zeigen, dass unsere Ergebnisse gut mit denen der Neutron Scattering Experimente vereinbar sind. KW - molecular dynamics KW - membrane adhesion KW - lipid-anchored saccharide KW - lipid membranes KW - membrane adhesion forces KW - Molekulardynamik KW - Membranadhäsion KW - lipid-verankerte Saccharide KW - Lipidmembran KW - Membran-Adhäsionskräfte Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-428790 ER - TY - THES A1 - Solopow, Sergej T1 - Wavelength dependent demagnetization dynamics in Co2MnGa Heusler-alloy T1 - Wellenlängeabhängige Entmagnetisierungsdynamik in Co2MnGa Heusler-Legierung N2 - In dieser Arbeit haben wir ultraschnelle Entmagnetisierung an einer Heusler-Legierung untersucht. Es handelt sich um ein Halbmetall, das sich in einer ferromagnetischen Phase befindet. Die Besonderheit dieses Materials besteht im Aufbau einer Bandstruktur. Diese bildet Zustandsdichten, in der die Majoritätselektronen eine metallische Bänderbildung aufweisen und die Minoritätselektronen eine Bandlücke in der Nähe des Fermi-Niveaus aufweisen, das dem Aufbau eines Halbleiters entspricht. Mit Hilfe der Pump-Probe-Experimente haben wir zeitaufgelöste Messungen durchgeführt. Für das Pumpen wurden ultrakurze Laserpulse mit einer Pulsdauer von 100 fs benutzt. Wir haben dabei zwei verschiedene Wellenlängen mit 400 nm und 1240 nm benutzt, um den Effekt der Primäranregung und der Bandlücke in den Minoritätszuständen zu untersuchen. Dabei wurde zum ersten Mal OPA (Optical Parametrical Amplifier) für die Erzeugung der langwelligen Pulse an der FEMTOSPEX-Beamline getestet und erfolgreich bei den Experimenten verwendet. Wir haben Wellenlängen bedingte Unterschiede in der Entmagnetisierungszeit gemessen. Mit der Erhöhung der Photonenenergie ist der Prozess der Entmagnetisierung deutlich schneller als bei einer niedrigeren Photonenenergie. Wir verknüpften diese Ergebnisse mit der Existenz der Energielücke für Minoritätselektronen. Mit Hilfe lokaler Elliot-Yafet-Streuprozesse können die beobachteten Zeiten gut erklärt werden. Wir haben in dieser Arbeit auch eine neue Probe-Methode für die Magnetisierung angewandt und somit experimentell deren Effektivität, nämlich XMCD in Refletiongeometry, bestätigen können. Statische Experimente liefern somit deutliche Indizien dafür, dass eine magnetische von einer rein elektronischen Antwort des Systems getrennt werden kann. Unter der Voraussetzung, dass die Photonenenergie der Röntgenstrahlung auf die L3 Kante des entsprechenden Elements eingestellt, ein geeigneter Einfallswinkel gewählt und die zirkulare Polarisation fixiert wird, ist es möglich, diese Methode zur Analyse magnetischer und elektronischer Respons anzuwenden. N2 - In this work we investigated ultrafast demagnetization in a Heusler-alloy. This material belongs to the halfmetal and exists in a ferromagnetic phase. A special feature of investigated alloy is a structure of electronic bands. The last leads to the specific density of the states. Majority electrons form a metallic like structure while minority electrons form a gap near the Fermi-level, like in semiconductor. This particularity offers a good possibility to use this material as model-like structure and to make some proof of principles concerning demagnetization. Using pump-probe experiments we carried out time-resolved measurements to figure out the times of demagnetization. For the pumping we used ultrashort laser pulses with duration around 100 fs. Simultaneously we used two excitation regimes with two different wavelengths namely 400 nm and 1240 nm. Decreasing the energy of photons to the gap size of the minority electrons we explored the effect of the gap on the demagnetization dynamics. During this work we used for the first time OPA (Optical Parametrical Amplifier) for the generation of the laser irradiation in a long-wave regime. We tested it on the FETOSPEX-beamline in BASSYII electron storage ring. With this new technique we measured wavelength dependent demagnetization dynamics. We estimated that the demagnetization time is in a correlation with photon energy of the excitation pulse. Higher photon energy leads to the faster demagnetization in our material. We associate this result with the existence of the energy-gap for minority electrons and explained it with Elliot-Yaffet-scattering events. Additionally we applied new probe-method for magnetization state in this work and verified their effectivity. It is about the well-known XMCD (X-ray magnetic circular dichroism) which we adopted for the measurements in reflection geometry. Static experiments confirmed that the pure electronic dynamics can be separated from the magnetic one. We used photon energy fixed on the L3 of the corresponding elements with circular polarization. Appropriate incidence angel was estimated from static measurements. Using this probe method in dynamic measurements we explored electronic and magnetic dynamics in this alloy. KW - magnetizationdynamic KW - XMCD KW - Heusler-alloy KW - Magnetisierungsdynamik KW - XMCD KW - Heusler-Legierung Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-427860 ER - TY - JOUR A1 - Sarhan, Radwan Mohamed A1 - Koopman, Wouter-Willem Adriaan A1 - Schuetz, Roman A1 - Schmid, Thomas A1 - Liebig, Ferenc A1 - Koetz, Joachim A1 - Bargheer, Matias T1 - The importance of plasmonic heating for the plasmondriven photodimerization of 4-nitrothiophenol JF - Scientific Reports N2 - Metal nanoparticles form potent nanoreactors, driven by the optical generation of energetic electrons and nanoscale heat. The relative influence of these two factors on nanoscale chemistry is strongly debated. This article discusses the temperature dependence of the dimerization of 4-nitrothiophenol (4-NTP) into 4,4′-dimercaptoazobenzene (DMAB) adsorbed on gold nanoflowers by Surface-Enhanced Raman Scattering (SERS). Raman thermometry shows a significant optical heating of the particles. The ratio of the Stokes and the anti-Stokes Raman signal moreover demonstrates that the molecular temperature during the reaction rises beyond the average crystal lattice temperature of the plasmonic particles. The product bands have an even higher temperature than reactant bands, which suggests that the reaction proceeds preferentially at thermal hot spots. In addition, kinetic measurements of the reaction during external heating of the reaction environment yield a considerable rise of the reaction rate with temperature. Despite this significant heating effects, a comparison of SERS spectra recorded after heating the sample by an external heater to spectra recorded after prolonged illumination shows that the reaction is strictly photo-driven. While in both cases the temperature increase is comparable, the dimerization occurs only in the presence of light. Intensity dependent measurements at fixed temperatures confirm this finding. KW - enhanced raman-scattering KW - charge-transfer KW - metal KW - nanoparticles KW - catalysis KW - AU KW - 4-nitrobenzenethiol KW - aminothiophenol KW - photocatalysis KW - wavelength Y1 - 2019 U6 - https://doi.org/10.1038/s41598-019-38627-2 SN - 2045-2322 VL - 9 PB - Macmillan Publishers Limited CY - London ER - TY - THES A1 - Cecchini, Gloria T1 - Improving network inference by overcoming statistical limitations T1 - Verbesserung der Netzwerkrekonstruktion durch überwinden statistischer Limits N2 - A reliable inference of networks from data is of key interest in many scientific fields. Several methods have been suggested in the literature to reliably determine links in a network. These techniques rely on statistical methods, typically controlling the number of false positive links, but not considering false negative links. In this thesis new methodologies to improve network inference are suggested. Initial analyses demonstrate the impact of falsepositive and false negative conclusions about the presence or absence of links on the resulting inferred network. Consequently, revealing the importance of making well-considered choices leads to suggest new approaches to enhance existing network reconstruction methods. A simulation study, presented in Chapter 3, shows that different values to balance false positive and false negative conclusions about links should be used in order to reliably estimate network characteristics. The existence of type I and type II errors in the reconstructed network, also called biased network, is accepted. Consequently, an analytic method that describes the influence of these two errors on the network structure is explored. As a result of this analysis, an analytic formula of the density of the biased vertex degree distribution is found (Chapter 4). In the inverse problem, the vertex degree distribution of the true underlying network is analytically reconstructed, assuming the probabilities of type I and type II errors. Chapters 4-5 show that the method is robust to incorrect estimates of α and β within reasonable limits. In Chapter 6, an iterative procedure to enhance this method is presented in the case of large errors on the estimates of α and β. The investigations presented so far focus on the influence of false positive and false negative links on the network characteristics. In Chapter 7, the analysis is reversed - the study focuses on the influence of network characteristics on the probability of type I and type II errors, in the case of networks of coupled oscillators. The probabilities of α and β are influenced by the shortest path length and the detour degree, respectively. These results have been used to improve the network reconstruction, when the true underlying network is not known a priori, introducing a novel and advanced concept of threshold. N2 - Eine zuverlässige Rekonstruktion eines Netzwerks aus Daten ist von entscheidender Bedeutung in der Wissenschaft. Einige Methoden werden in der Literatur vorgeschlagen um Verbindungen in einem Netzwerk akkurat zu bestimmen. Diese Methoden vertrauen auf die Anwendung der Statistik, indem sie falsch positive Verbindungen berücksichtigen, allerdings positiv falsche Verbindungen ignoriert. In dieser Arbeit werden neue Methoden vorgeschlagen, um die Rekonstruktion zu verbessern. Erste Analysen veranschaulichen den Einfluss falsch positiver und positiv falscher Verbindungen auf das resultierende Netzwerk. Daraus wird die Bedeutsamkeit ersichtlich, die eine gut gewählte Entscheidung hinsichtlich der Faktoren auf die Qualität der Rekonstruktion hat, wodurch sich neu Methoden ableiten lassen. Eine Simulation, welche in Kapitel 3 zu finden ist, veranschaulicht, dass verschiedene Werte für falsch postive und positiv falsche Verbindungen zu verwenden sind, um genaue Vorhersagen bezüglich des Netzwerkverhaltens zu treffen. Die Existenz Fehler erster und zweiter Art in der Rekonstruktion sind unvermeidbar und werden akzeptiert. Ein analytischer Ansatz, der den Einfluss dieser beiden Fehler beschreibt wird gesucht. Aus dieser Analyse in Kapitel 4 folgt eine Formel welche die Verteilung der Quantität der Knotenverbindungen beschreibt. Bei dem inversen Problem wird die Knotengrad-Verteilung des originalen Netzwerkes, mit Berücksichtigung der Wahrscheinlichkeit von Fehlern erster und zweiter Art, analytisch berechnet. Kapitel 4-5 zeigen, dass die Methode auch bei einigermaßen falschen Schätzungen von α und β Resultate innerhalb vertretbarer Grenzen liefert. In Kapitel 6 wird ein iteratives Verfahren vorgestellt, welches diese Methode bei außerordentlich falschen Schätzungen von α und β verbessert. Die bis jetzt vorgestellte Recherche fokussiert sich auf den Einfluss falsch positiver und positiv falscher Verbindungen auf die Netzwerkscharakteristik. Im Kapitel 7 wird der Prozess umgedreht. Die Arbeit fokussiert sich auf den Einfluss auf die Netzwerkkarakteristik durch die Fehler erster und zweiter Art im Falle eines Netzwerkes mit gekoppelten Oszillatoren. Die Wahrscheinlichkeit von α und β wird beeinflusst durch den kürzesten Verbindungsweg und dem Detour Grad. Diese Ergebnisse wurden genutzt um die Netzwerk Rekonstruktion zu verbessern, wenn das originale Netzwerk nicht zuvor bekannt war. Dies beschreibt einen neuen fortgeschritten Weg der Grenzwertbestimmung. KW - network inference KW - network reconstruction KW - statistical methods KW - Netzwerk Inferenz KW - Netzwerk Rekonstruktion KW - statistische Methoden Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-426705 ER - TY - THES A1 - Kegelmann, Lukas T1 - Advancing charge selective contacts for efficient monolithic perovskite-silicon tandem solar cells T1 - Entwicklung Ladungsselektiver Kontakte für Effiziente Monolithische Perowskit-Silizium Tandem-Solarzellen N2 - Hybrid organic-inorganic perovskites are one of the most promising material classes for photovoltaic energy conversion. In solar cells, the perovskite absorber is sandwiched between n- and p-type contact layers which selectively transport electrons and holes to the cell’s cathode and anode, respectively. This thesis aims to advance contact layers in perovskite solar cells and unravel the impact of interface and contact properties on the device performance. Further, the contact materials are applied in monolithic perovskite-silicon heterojunction (SHJ) tandem solar cells, which can overcome the single junction efficiency limits and attract increasing attention. Therefore, all contact layers must be highly transparent to foster light harvesting in the tandem solar cell design. Besides, the SHJ device restricts processing temperatures for the selective contacts to below 200°C. A comparative study of various electron selective contact materials, all processed below 180°C, in n-i-p type perovskite solar cells highlights that selective contacts and their interfaces to the absorber govern the overall device performance. Combining fullerenes and metal-oxides in a TiO2/PC60BM (phenyl-C60-butyric acid methyl ester) double-layer contact allows to merge good charge extraction with minimized interface recombination. The layer sequence thereby achieved high stabilized solar cell performances up to 18.0% and negligible current-voltage hysteresis, an otherwise pronounced phenomenon in this device design. Double-layer structures are therefore emphasized as a general concept to establish efficient and highly selective contacts. Based on this success, the concept to combine desired properties of different materials is transferred to the p-type contact. Here, a mixture of the small molecule Spiro-OMeTAD [2,2’,7,7’-tetrakis(N,N-di-p-methoxyphenylamine)-9,9’-spirobifluoren] and the doped polymer PEDOT [poly(3,4-ethylenedioxythiophene)] is presented as a novel hole selective contact. PEDOT thereby remarkably suppresses charge recombination at the perovskite surface, allowing an increase of quasi-Fermi level splitting in the absorber. Further, the addition of Spiro-OMeTAD into the PEDOT layer is shown to enhance charge extraction at the interface and allow high efficiencies up to 16.8%. Finally, the knowledge on contact properties is applied to monolithic perovskite-SHJ tandem solar cells. The main goal is to optimize the top contact stack of doped Spiro-OMeTAD/molybdenum oxide(MoOx)/ITO towards higher transparency by two different routes. First, fine-tuning of the ITO deposition to mitigate chemical reduction of MoOx and increase the transmittance of MoOx/ITO stacks by 25%. Second, replacing Spiro-OMeTAD with the alternative hole transport materials PEDOT/Spiro-OMeTAD mixtures, CuSCN or PTAA [poly(triaryl amine)]. Experimental results determine layer thickness constrains and validate optical simulations, which subsequently allow to realistically estimate the respective tandem device performances. As a result, PTAA represents the most promising replacement for Spiro-OMeTAD, with a projected increase of the optimum tandem device efficiency for the herein used architecture by 2.9% relative to 26.5% absolute. The results also reveal general guidelines for further performance gains of the technology. N2 - Hybride, organisch-anorganische Perowskite gelten als eine der vielversprechendsten Materialklassen für die photovoltaische Energieumwandlung. Dazu werden Perowskit-Absorber in Solarzellen zwischen n- und p-Typ Kontaktschichten angeordnet, die Elektronen oder Löcher selektiv zur Kathode bzw. Anode der Zelle transportieren. Ziel dieser Arbeit ist es, die ladungsselektiven Transportschichten in Perowskit-Solarzellen zu verbessern und Einflüsse der Grenzflächen- und Kontakteigenschaften auf die Zelleffizienz herauszustellen. Darüber hinaus werden die selektiven Schichten in monolithischen Perowskit-Silizium-Heterokontakt (SHK) Tandem-Solarzellen eingesetzt. Diese können höhere Wirkungsgrade als Einfachsolarzellen erzielen und erfahren zunehmende Aufmerksamkeit aus der Forschung. Hierfür müssen alle Kontaktschichten hochtransparent sein, um eine möglichst effiziente Lichtausnutzung im Tandem-Solarzellen-Design zu erzielen. Des Weiteren limitiert die SHK-Solarzelle die höchst mögliche Temperatur zur Abscheidung der selektiven Kontakte auf 200°C. In einer Vergleichsstudie werden deshalb zunächst verschiedene elektronenselektive Kontaktmaterialien, die alle unter 180°C prozessiert werden, in n-i-p-Typ Perowskit-Solarzellen eingesetzt. Es zeigt sich hierbei, wie wesentlich die selektiven Kontakte und ihre Grenzflächen zum Absorber die Effizienz der Solarzellen bestimmen. Eine Kombination aus Fulleren und Metalloxid in einem TiO2/PC60BM (Phenyl-C60-Buttersäuremethylester) Doppelschichtkontakt ermöglicht dabei eine besonders gute Ladungsextraktion und stark reduzierte Grenzflächenrekombination. Die Materialzusammenstellung erreicht in der Studie hohe stabilisierte Solarzellenwirkungsgrade bis zu 18,0% und eine vernachlässigbare Strom-Spannungs-Hysterese, ein üblicherweise ausgeprägtes Phänomen in diesem Zellaufbau. Das Ergebnis stellt Doppelschicht-Strukturen als generelles Konzept zur Herstellung effizienter und hochselektiver Kontakte heraus. Basierend auf diesem Erfolg wird das Konzept, Eigenschaften verschiedener Materialien miteinander zu kombinieren, anschließend auf den p-Typ Kontakt übertragen. Dazu wird ein neuartiger lochselektiver Kontakt vorgestellt, bestehend aus einer Mischung des kleinen Moleküls Spiro-OMeTAD [2,2‘7,7‘-tetrakis(N,N-di-p-methoxyphenylamin)-9,9‘-spirobifluoren] und dem dotierten Polymer PEDOT [poly(3,4-ethylendioxythiophen)]. PEDOT unterdrückt dabei bemerkenswerter Weiße die Ladungsträgerrekombination an der Perowskit-Grenzfläche, wodurch eine Erhöhung der Quasi-Fermi-Niveau-Aufspaltung im Absorber erzielt wird. Weiterhin wird gezeigt, dass die Zugabe von Spiro-OMeTAD in die PEDOT-Schicht die Lochextraktion an der Grenzfläche verbessert und folglich hohe Solarzellenwirkungsgrade von bis zu 16,8% ermöglicht. Schließlich wird das gewonnene Wissen über die Bedeutung der Kontakt- und Grenzflächeneigenschaften auf monolithische Perowskit-SHK-Tandemsolarzellen angewandt. Das Hauptziel dabei ist die Optimierung des oberen Kontaktstapels, bestehend aus dotiertem Spiro-OMeTAD/Molybdän Oxid (MoOx)/ITO, hin zu verbesserter Transparenz. Zwei verschiedene Ansätze werden hierzu verfolgt. Erstens, durch Feinanpassung der ITO-Abscheidung kann eine chemische Reduktion von MoOx verringert und die Transmission von MoOx/ITO-Schichtstapeln um 25% erhöht werden. Zweitens: Durch Ersetzen des Spiro-OMeTAD mit alternativen, transparenteren Lochtransportmaterialien sollen parasitäre Absorptionsverluste vermieden werden. Als potentielle Lochkontakte werden dabei PEDOT/Spiro-OMeTAD-Mischungen, CuSCN und PTAA [Poly(triarylamin)] analysiert. Experimentelle Untersuchungen liefern optimierte Dicken der Lochkontakt und MoOx Schichten und dienen der Validierung optischer Simulationen der Schichtstapel. Dies erlaubt im Folgenden eine realistische Abschätzung der maximal erreichbaren Tandemsolarzelleneffizienzen. Dabei stellt PTAA den vielversprechendsten Ersatz für Spiro-OMeTAD dar, mit einer prognostizierten Erhöhung des erreichbaren Tandem-Solarzellenwirkungsgrad um 2,9% relativ auf 26,5% absolut. Die Ergebnisse stellen zudem einen Leitfaden zur weiteren Effizienzsteigerung der Tandemsolarzellen-Technologie dar. KW - perovskite KW - silicon KW - tandem solar cell KW - interface engineering KW - contact layers KW - Perowskit KW - Silizium KW - Tandem-Solarzelle KW - Interface-Engineering KW - Kontaktschichten Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-426428 ER - TY - THES A1 - Eckert, Sebastian T1 - Accessing active sites of molecular proton dynamics N2 - The unceasing impact of intense sunlight on earth constitutes a continuous source of energy fueling countless natural processes. On a molecular level, the energy contained in the electromagnetic radiation is transferred through photochemical processes into chemical or thermal energy. In the course of such processes, photo-excitations promote molecules into thermally inaccessible excited states. This induces adaptations of their molecular geometry according to the properties of the excited state. Decay processes towards energetically lower lying states in transient molecular geometries result in the formation of excited state relaxation pathways. The photo-chemical relaxation mechanisms depend on the studied system itself, the interactions with its chemical environment and the character of the involved states. This thesis focuses on systems in which photo-induced deprotonation processes occur at specific atomic sites. To detect these excited-state proton dynamics at the affected atoms, a local probe of molecular electronic structure is required. Therefore, site-selective and orbital-specific K-edge soft X-ray spectroscopy techniques are used here to detect photo-induced proton dynamics in gaseous and liquid sample environments. The protonation of nitrogen (N) sites in organic molecules and the oxygen (O) atom in the water molecule are probed locally through transitions between 1s orbitals and the p-derived molecular valence electronic structure. The used techniques are X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Both yield access to the unoccupied local valence electronic structure, whereas the latter additionally probes occupied states. We apply these probes in optical pump X-ray probe experiments to investigate valence excited-state proton transfer capabilities of aqueous 2-thiopyridone. A characteristic shift of N K-edge X-ray absorption resonances as well as a distinct X-ray emission line are established by us as spectral fingerprints of N deprotonation in the system. We utilize them to identify photo-induced N deprotonation of 2-thiopyridone on femtosecond timescales, in optical pump N K-edge RIXS probe measurements. We further establish excited state proton transfer mechanisms on picosecond and nanosecond timescales along the dominant relaxation pathways of 2-thiopyridone using transient N K-edge XAS. Despite being an excellent probe mechanism for valence excited-state proton dynamics, the K-edge core-excitation itself also disturbs the electronic structure at specific sites of a molecule. The rapid reaction of protons to 1s photo-excitations can yield directional structural distortions within the femtosecond core-excited state lifetime. These directional proton dynamics can change the energetic separation of eigenstates of the system and alter probabilities for radiative decay between them. Both effects yield spectral signatures of the dynamics in RIXS spectra. Using these signatures of RIXS transitions into electronically excited states, we investigate proton dynamics induced by N K-edge excitation in the amino-acid histidine. The minor core-excited state dynamics of histidine in basic and neutral chemical environments allow us to establish XAS and RIXS spectral signatures of different N protonation states at its imidazole N sites. Based on these signatures, we identify an excitation-site-independent N-H dissociation for N K-edge excitation under acidic conditions. Such directional structural deformations, induced by core-excitations, also make proton dynamics in electronic ground states accessible through RIXS transitions into vibrationally excited states. In that context, we interpret high resolution RIXS spectra of the water molecule for three O K-edge resonances based on quantum-chemical wave packet propagation simulations. We show that highly oriented ground state vibrational modes of coupled nuclear motion can be populated through RIXS processes by preparation of core-excited state nuclear wave packets with the same directionality. Based on that, we analytically derive the possibility to extract one-dimensional directional cuts through potential energy surfaces of molecular systems from the corresponding RIXS spectra. We further verify this concept through the extraction of the gas-phase water ground state potential along three coordinates from experimental data in comparison to quantum-chemical simulations of the potential energy surface. This thesis also contains contributions to instrumentation development for investigations of photo-induced molecular dynamics at high brilliance X-ray light sources. We characterize the setup used for the transient valence-excited state XAS measurements of 2-thiopyridone. Therein, a sub-micrometer thin liquid sample environment is established employing in-vacuum flat-jet technology, which enables a transmission experimental geometry. In combination with a MHz-laser system, we achieve a high detection sensitivity for photo-induced X-ray absorption changes. Additionally, we present conceptual improvements for temporal X-ray optical cross-correlation techniques based on transient changes of multilayer optical properties, which are crucial for the realization of femtosecond time-resolved studies at synchrotrons and free-electron lasers. N2 - Die stetige Bestrahlung der Erde mit intensivem Sonnenlicht stellt einen permanente Energiequelle dar, die zahllose natürliche Prozesse antreibt. Auf molekularer Ebene wird die Energie der elektromagnetischen Strahlung durch photochemische Prozesse in chemische und thermische Energie umgewandelt. Während dieser Prozesse werden thermisch nicht erreichbare angeregte Zustände von Molekülen durch Photoanregungen bevölkert. Dies führt zu Änderungen der Molekülgeometrie, die abhängig von den Eigenschaften der angeregten Zustände sind. Zerfallsprozesse in energetisch tieferliegende Zustände in transienten Molekülgeometrien führen zur Ausbildung von Relaxationspfaden angeregter Zustände. Die Relaxationsmechanismen sind dabei abhängig vom untersuchten System selbst, den Wechselwirkungen mit seiner chemischen Umgebung und den Eigenschaften der beteiligten angeregten Zustände. In dieser Arbeit werden Systeme untersucht, in denen die Protonierung bestimmter Atome im Molekül durch eine Photoanregung geändert werden kann. Um Protonendynamik an den betreffenden Atomen zu untersuchen, wird ein lokaler Zugang zur elektronischen Struktur des Moleküls benötigt. Daher wird in dieser Arbeit K-Kanten Weichröntgenspektroskopie genutzt, um photo-induzierte Protonendynamik in gasförmigen und flüssigen Proben zu untersuchen. Zusätzlich zur Selektivität bzgl. des Elements und des chemischen Zustands des betreffenden Atoms bietet diese Zugang zum Charakter und zur Lokalisierung der bindungsformenden Valenzorbitale. Die Protonierung von Stickstoffatomen (N) in organischen Systemen und die des Sauerstoffatoms (O) im Wassermolekül wird dabei durch Übergänge zwischen stark lokalisierten 1s- und Valenzorbitalen mit 2p-Charakter detektiert. Die verwendeten Spektroskopiemethoden Röntgenabsorption (engl. X-ray absorption spectroscopy, XAS) und resonate inelastische Röntgenstreuung (engl. resonant inelastic X-ray scattering, RIXS) bieten dabei einen lokalen Zugang zur unbesetzten bzw. im Fall von RIXS auch zur besetzten elektronischen Struktur der untersuchten Moleküle. Mit Hilfe der genannten Methoden haben wir in zeitaufgelösten Anrege-Abfrage (engl. pump-probe) Experimenten durch Valenzanregungen induzierte Protonentransfer-Prozesse (engl. excited state proton transfer, ESPT) des Moleküls 2-Thiopyridon in wässriger Lösung untersucht. Eine Verschiebung der N K-Kanten Röntgenabsorptionsresonanzen, sowie eine charakteristische Röntgenemissionslinie werden von uns als spektrale Signaturen einer N Deprotonierung des Systems etabliert. Eine potenzielle photo-induzierte N Deprotonierung des Moleküls wird anhand dieser Signaturen auf femtosekunden Zeitskalen über zeitaufgelöste N K-Kanten RIXS Messungen identifiziert. Protonentransfer-Mechanismen auf Pico- und Nanosekunden Zeitskalen entlang der dominanten Relaxationspfade des Systems werden mit zeitaufgelöstem N K-Kanten XAS untersucht. K-Kanten Rumpfanregungen eignen sich nicht nur ideal zur Detektion von Protonendynamik in valenzangeregten Zuständen, da die Rumpfanregungen selbst auch eine lokalisierte Störung der elektronischen Struktur darstellen. Vor allem die Reaktion von Protonen auf diese Störung innerhalb der 1s Rumpfloch-Lebensdauer von wenigen Femtosekunden kann zu einer gerichteten Verzerrung der Molekülstruktur führen. Die damit verbundenen Änderungen von Übergangsenergien und -wahrscheinlichkeiten sind als Signaturen dieser gerichteten Protonendynamik in RIXS Spektren zugänglich. Anhand von RIXS Übergängen in elektronisch angeregte Zustände untersuchen wir Protonendynamik, die durch N K-Kanten Anregungen an den N Atomen im Imidazolring der Aminosäure Histidin induziert wird. Die schwache Dynamik in basischen und neutralen wässrigen Lösungen erlauben es uns, die Protonierung dieser N Atome mit charakteristischen spektralen Signaturen zu korrelieren. Mit Hilfe dieser Signaturen identifizieren wir eine durch K-Kanten Anregung verursachte N-H Dissoziation in saurer Lösung. Dieser Prozess ist unabhängig davon, an welchem der N Atome des Imidazolrings die Rumpfanregung lokalisiert ist. Solche, durch Rumpfanregungen verursachten, gerichteten Verzerrungen der Molekülstruktur ermöglichen einen Zugang zu Protonendynamik im elektronischen Grundzustand über RIXS Prozesse in dessen vibrationsangeregte Zustände. In diesem Zusammenhang vergleichen wir hochaufgelöste O K-Kanten RIXS Spektren des Wassermoleküls in der Gasphase mit quantenchemischen Simulationen zur Wellenpaketpropagation in den rumpfangeregten Zuständen. Dabei wird deutlich, dass die gerichtete Verzerrung der Molekülstruktur im rumpfangeregten Zustand eine Bevölkerung von Vibrationsmoden des Grundzustandes mit der gleichen Ausrichtung durch den RIXS Prozess verursacht. Anhand dieser Ergebnisse leiten wir ab, unter welchen Bedingungen eine Extraktion eindimensionaler Querschnitte der Potentialfläche des Grundzustandes aus den entsprechenden RIXS Spektren möglich ist. Wir verifizieren diese Methode anhand der Extraktion der Grundzustandspotentialfläche des Wassermoleküls entlang drei unterschiedlicher Richtungen im Vergleich zu den quantenchemischen Rechnungen. Diese Arbeit enthält zudem Beiträge zur Entwicklung von Instrumentierung für Untersuchungen valenzangeregter Moleküldynamik an Röntgenquellen mit hoher Brillianz. Der experimentelle Aufbau, der für die zeitaufgelösten XAS Messungen an 2-Thiopyridon verwendet wurde, wird vorgestellt. Ein sub-Mikrometer dünner Flüssigkeitsflachstrahl erlaubt dabei Messungen in einer Transmissionsgeometrie. In Kombination mit einem MHz-Lasersystem können transiente Absorptionsänderungen effizient detektiert werden. Zudem präsentieren wir Konzepte zur zeitlichen Korrelation von Röntgen- und optischen Lichtpulsen, basierend auf Änderungen der optischen Eigenschaften von Dünnschichtsystemen, die essenziell für Studien transienter Prozesse an Synchrotrons und Freie-Elektronen Lasern mit Femtosekunden Zeitauflösung sind. KW - molecular proton dynamics KW - Protonendynamik molekularer Systeme KW - K-edge soft X-ray spectroscopy KW - K-Kanten Weichröntgenspektroskopie KW - excited state proton transfer KW - Protonentransfer in angeregten Zuständen KW - core-excited state dynamics KW - Dynamik in rumpfangeregten Zuständen KW - optical pump - X-ray probe spectroscopy KW - Kurzzeitspektroskopie mit optischer Anregung und Röntgendetektion Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-425870 ER -